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The past and future of sustainable concrete: A critical review and new
strategies on cement-based materials

Article in Journal of Cleaner Production · September 2020

DOI: 10.1016/j.jclepro.2020.123558

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 1 https://www.sciencedirect.com/science/article/pii/S0959652620336039

2
3 aCERIS, Civil Engineering, Architecture and Georresources Department, Instituto Superior Técnico, Universidade de Lisboa,
4 Av. Rovisco Pais, 1049-001 Lisbon, Portugal
5 bDepartment of Civil Engineering, Technical Engineering College, Erbil Polytechnic University, Erbil, Kurdistan-Region, Iraq
6 cScientific Research and Development Center, Nawroz University, Duhok, Kurdistan-Region, Iraq
7 Corresponding authors: jb@civil.ist.utl.pt (JB); Rawaz.kurda@epu.edu.iq (RK)

8 Abstract

9 The negative impacts of cement-based material (CBM) production are way bigger than ever expected.
10 To illustrate the scale of this phenomenon, all the forests in the world, regardless of the fact that they
11 are disappearing at an alarming rate, are not enough to offset even half the environmental impact (EI)
12 of global aggregates and cement production. Thus, it is necessary to promote scientific research and
13 guide more researchers and professionals in the construction industry to investigate the undiscovered
14 sustainability paths, namely for concrete before and after end-of-life. For that purpose, a global and
15 extensive review is made here to provide an overall view of concrete sustainability in all possible paths.
16 Then, each path is organized as follows: (i) brief introduction, (ii) presentation of non-traditional mate-
17 rials and techniques that can be used for the selected strategy, (iii) their limitations and (iv) future trends.
18 The study also identifies what is already known to avoid putting valuable research resources into redun-
19 dant scientific studies. The following paths of concrete production sustainability were identified: mix
20 composition (e.g. reduce the EI and resources use of binders, aggregates, water and reinforcement),
21 materials manufacturing (e.g. new production techniques of cement, aggregates and steel bars), con-
22 crete mixing (e.g. mixer type and mixing method), on-site application (e.g. regular casting and digital
23 concrete/3D printing), and in-service performance (e.g. increase the durability of reinforced concrete
24 and carbon capture and thermal conductivity). On most of these paths, many studies have been made
25 on the same non-traditional materials and techniques and similar outputs were obtained. Yet, many
26 other non-traditional materials and techniques have not been explored before, or are incomplete in
27 terms of the characteristics analysed. More than providing definite solutions, this contribution intends
28 to open the minds of the readers to the vastly unexplored world of “green concrete”.

1
29 Main Keywords

30 Concrete sustainability; Life-cycle assessment; Cementitious materials; Recycled materials; Sustainable

31 development; Integrated sustainability trends.

32 Acronyms list:

AAM - Alkali-activated material MIBA - municipal solid waste incinerator bottom ash
ACR - alkali-carbonate reaction MIFA - municipal solid waste incinerator fly ash
ADP - abiotic depletion potential MRA - mixed recycled aggregate
AP - acidification potential MSA - mussel shell ash
ASR - alkali-silica reaction NF - natural fibres
AWA - agricultural waste ash ODP - ozone depletion potential
AWAF - agricultural wastes and aquaculture farming OPC - Ordinary Portland cement
AWAFA - agricultural wastes and aquaculture farming ashes OWA - olive waste ash
BLA - bamboo leaf ash PCM - Phase change materials
BTQ - binary, ternary and quaternary PE-NRe - non-renewable primary energy resources
CBA - coal bottom ash PE-Re - renewable primary energy resources
CBM - cement-based materials POCP - photochemical ozone creation potential
CCA - corn cob ash POFA - palm oil fuel ash
CDRA - mixed construction and demolition recycled aggregate RCA - recycled concrete aggregate
CDW - construction and demolition waste RH - rise husk; RHA - rise husk ash
CNT - carbon nanotubes RMA - recycled masonry aggregate
ECR - epoxy-coated rebar SAP - Super absorbent polymer
EC - expanded clay SA - silica aerogel
ECG - expanded cork granules SBA - sugarcane bagasse ash
EGA - elephant grass ash SCC - self-compacting concrete
EI - environmental impacts SCM - supplementary cementitious material
EP - Eutrophication potential SF - silica fume
FA - coal fly ash SMM - Shape memory material
FBBA - forest biomass bottom ash SP - Superplasticizer
FRP - fibre reinforced-polymer SSA - sewage sludge ash
GGBS - ground granulated blast furnace slag SSD - saturated surface-dry
GR - galvanized rebars SSR - stainless steel rebar
GWP - Global warming potential TWA - tire waste aggregate
L - lime TWA - tobacco waste ash
LCA - Life Cycle Assessment WA - wood ashes
LOI - loss on ignition w/b - water to binder ratio
LWA - light-weight aggregate WFA - wood fly ash
M - methylcellulose WSA- wheat straw ash
33

34

35

2
36 1 Introduction

37 Many studies have alerted us to the negative impacts of cement-based materials (CBM) production
38 within the construction industry. These impacts may be way bigger than ever anticipated. Illustrating the
39 concept, the total world production of aggregates and cement can be around 48.3 billion tonnes [1, 2]
40 and 4.1 billion tonnes (average - [3, 4]) in 2018, respectively. Additionally, the average global warming
41 potential (GWP) of 1 kg aggregate and cement is 0.0123 kg CO2 eq [5-8] and 0.981 kg CO2 eq [5, 8-13],
42 respectively. Thus, the total GWP of aggregates and cement will be around 5.9409E+11 kg CO2 eq and
43 4.0221E+12 kg CO2 eq, respectively. Contrary to a common statement, instead of concrete, aggregates
44 are the most consumed material after water. Previous values shown in the previous sentences indicate
45 that, although aggregates consumption is almost 12 times bigger than that of cement, their environmen-
46 tal impact (EI) is insignificant relatively to cement. If one considers all of the produced aggregates and
47 cement used for paste, mortar and concrete without considering the mixing procedure and transporta-
48 tion, the total GWP will be around 4.61373E+12 kg CO2 eq. Thus, the EI of the main raw materials to
49 produce paste, mortar and concrete is at least 1.6 times higher than the total emitted CO2 by “human
50 exhalation” and corresponds to 7% of “all human activities including exhalation” per year (source of the
51 secondary data: human population ≈ 7.7576E+09 [14], global normalisation factors for the environmen-
52 tal footprint and Life Cycle Assessment - LCA of all activities of human [15] per year ≈ 8.40E+03 kg CO2
53 eq, Human CO2 exhalation [16] per year ≈ 365 kg CO2 eq). Furthermore, the CO2 emission of aggregates
54 and cement production is about 7% of the total CO2 absorbance by the three trillion trees on the surface
55 of Earth (source of the secondary data: number of trees ≈ three trillion [17] and CO2 consumption of a
56 mature tree ≈ 22 kg/year [18]). As a result, we can say that if it were not for some tiny ocean plants,
57 namely phytoplankton, the total trees on our planet would not be enough to offset all human activities.

58 Most of the materials used in concrete production are, in sensu stricto, non-sustainable because they
59 are coming from non-renewable sources. In addition, concrete may contribute to 4-8% of the world’s
60 CO2 and consume a significant amount of natural resources, besides other negative impacts during con-
61 crete mixing and on-site application. Nevertheless, the term sustainability mentioned in this work, can
62 still be used to characterize the concrete production, since concrete is one of the most competitive con-
63 struction materials and it can last for centuries. In fact, concrete is arguably the main driver of modern
64 development, protecting humans from natural disasters and providing a structure for transportation,
65 education, healthcare, energy, among many other industries.

66 After an extensive review, the lessons learned show that many case studies and review studies have been
67 made to overcome the mentioned issue regarding the high negative impact of the construction industry,

3
68 namely that of concrete. For example, similarly to this study, there are other attempts focused the gate-
69 to-cradle boundaries of CBM [19] and concrete pavements [20] in the construction industry, including
70 the relationship between the main sustainability parameters (e.g. cost and performance, including
71 rehabilitation cost, versus service life for high- and low- performance concrete). Nevertheless, to the
72 best of the authors’ knowledge, there is no single study collecting all the strategies (given example for each)
73 and providing a global overview of the mix design and whole life cycle of concrete (Figure 1), namely mix
74 composition (sections 3-7), materials manufacturing (section 8), concrete mixing (section 9), on-site appli-
75 cation (section 10) and in-service performance (sections 11-13). Thus, this study organized and discussed
76 most of the potential strategies to guide and introduce scientists and the general public in and outside the
77 construction industry to the available sustainability options. Apart from introducing the most sustainable
78 options for CBM, this study also shows the limitations (critical issues) and future needed investigation for
79 these strategies to be a baseline and foundation for coming studies.

4
 Sections 3-7:
Mix composition Reduce the total amount of binder
Reduce the EI and resource use of binders
Reduce the EI and resource use of water
Reduce the EI of aggregates
Reduce the EI of reinforcement

Section 8:
Materials
manufacturing Cement production
Aggregates production
Production of reinforcement
Production of water
Production of other materials (e.g. superplasticizer)

End of life Concrete mixing Section 9:

Types of mixer Mixing method

Section 10:
Pre-construction and pre-placement meetings
Concrete ordering procedures
Transporting and receiving concrete
Conveying, placing, consolidating and finishing concrete
Concrete protection and curing requirements
In-service On site
performance application Sections 11-13:
Increase the durability of reinforced concrete
CO₂ mineralization and utilization
Thermal conductivity improvement and energy saving
80

81 Figure 1 - Strategies for sustainable concrete

5
 82 2 Methodology

83 This work is a systematic and extensive analysis that intends to synthesize, identify, and evaluate the
84 literature regarding the sustainability paths concerning mix design and whole life cycle of CBM (Figure
85 1), with special emphasis on concrete. Thereafter, this work is followed by an exhaustive analysis of
86 the literature to identify topics for further study. The study is mainly focused on the various options
87 to move towards CBM’s sustainability. Thus, a literature research was made using the search engines
88 of several databases (Figure 2). For each database, the same search options were repeated using com-
89 binations of different keywords based on the strategy. Furthermore, for each selected study, the ref-
90 erence list and the studies cited in the selected study were checked to find further relevant studies.

Search in:
Any, topic,
title, articles Google
with author Scholar
supplied
Document keywords
Data range:
type: Article, Scopus ScienceDirect
from past to
Review,
January,
conference Search 2020
papers
options Databases
Article types: Web of Research
Review Science Gate
Language:
articles,
Mostly
research Taylor and
English
articles, data Francis
paper
91
92 Figure 2 - Databases and search options (besides the main databases, other databases such as ICE, Wiley
93 Online Library, RILEM, Web of Knowledge are also considered)

94 Since the range of the study is very wide and the number of cited references is unusual, various strict bound-
95 aries were defined to maintain the reliability of the cited references (e.g. rank of the journal, number of
96 citations and number of the studied parameters and samples). The validity of the selected papers was spec-
97 ified by analysing the title, abstract, materials and methodology of the research studies. Thereafter, the non-
98 relevant studies were removed. For that purpose, several main criteria were defined in order to demon-
99 strate whether a material is relevant to this research work. The chosen studies met the following criteria:

100 - For the scientific publications, the number of citations must be at least four except if it is
101 published in an ISI (Web of Science) journal or in a recent year;

102 - If there are many studies on the same strategy/subject, priority was given to those with more

6
103 complete parameters (e.g. considering EI, technical performance and cost);

104 - Review studies were prioritized relative to case studies;

105 - Finally, more recent studies were preferred to older publications;

106 - The focus is mostly on the studies that relate to concrete, followed by mortar and paste.

107 In some cases, the authors have use more than 3-4 references for a single path in order to stress that path
108 has been studied by multiple scholars, and researchers must avoid duplicating paths. In other cases, only a
109 few studies (e.g. 1-2 studies) have been used because the number of studies for that path is limited. The
110 basic body of the literature comprised 2,044 studies. The journal papers have the lion share of the total
111 number of cited studies (87%) and are distantly followed by conference papers (3%), book/book chapter
112 (3%), scientific reports (2%), standards (2%), theses (2%) and others (1%) such as patents, software, inter-
113 national symposiums/seminars and web-sites (Figure 3a). The ‘’publication and accessed year’’ of the ref-
114 erences range from 1956 to 2020 and 91% of the studies were made in the 2000-2020 period (Figure 3b).
115 Figure 4 shows the citations and publication year of the journal papers. Since there was a big gap between
116 the citation of the studies (e.g. 16, 64, 256, 1024 and 4096 citations), the scale was depicted in a different
117 manner (logarithmic scale). The results show that about 90% of the papers have at least four citations.

100% 87% 35% 33%

31%
References (%)

30%
References (%)

80%
25%
60% 20% 17%
40% 15% 10%
10%
20% 4%
1% 2% 2% 2% 3% 3% 5% 1% 2% 2%
0% 0%

118 (a) Publication type (b) Year

119 Figure 3 - Breakdown of cited references per publication (a) type and (b) year

120 Based on the citation number, the sections can be ordered as the following: sections 13, 12, 11, (6-10), 5, 4
121 and 3 (Figure 4). In general, section 13 (thermal conductivity improvement and energy saving) has received
122 the most citations, followed by section 12 (CO₂ mineralization and utilization) and then section 11 (increase
123 the durability of reinforced concrete) with a big scatter due to the wide scope of this section and many
124 studies on this path (Figure 5). After that, sections 6, 7, 8, 9 and 10 followed and they have similar citation
125 levels. Then came sections 5 (reduce the environmental impacts and resources use of aggregates) and 4
126 (reduce the environmental impacts and resources use of binders). Similarly to section 11, section 4 has a big

7
127 scatter due to its wide scope many studies on this path (Figure 5). Finally, studies relating to section 3 (reduce
128 the total amount of binder) had the least citations compared to other sections, probably due to the fact that
129 studies on this path are not majorly promoted by the scientific community and concrete industry. According
130 to Figure 5, about 73% of the studies relate to only sections 4-5 and 11. This means that most of the
131 efforts have been made on only a few sustainability paths and the others have been disregarded and
132 insufficiently developed.

4096
Section 3

Section 4
1024
Section 5
Citations number

Section 6
256
Section 7

Section 8
64
Section 9

Section 10
16
Section 11

Section 12
4
Section 13

1
1980 1985 1990 1995 2000 2005 2010 2015 2020
Year
133

134 Figure 4 - Publication year versus citations

Section 11 - Increase the durability of reinforced concrete 30%

Section 4 - Reduce the environmental impacts and resources use… 25%
Section 5 - Reduce the environmental impacts and resources use… 18%
Section 7 - Reduce the environmental impacts and resources use… 9%
Section 13 - Thermal conductivity improvement and energy saving 8%
Section 3 - Reduce the total amount of binder 7%
Section 8 - Material manufacturing 5%
Section 12 - CO₂ mineralization and utilization 3%
Section 6 - Reduce the environmental impacts and resources use… 1%
Section 10 - On-site application 1%
Section 9 - Concrete mixing 1%
0% 10% 20% 30%

135 References (%)

136 Figure 5 - Percentage of total cited papers per section

8
137 3 Reduce the total amount of binder

138 The essential goal of this strategy is to obtain environmental-friendly, durable and economically feasible
139 concrete mixes using an unconventionally low binder content. According to EN 206-1 [21], the minimum
140 cement content in concrete must be equal to or higher than 260 kg/m3 to achieve an adequate durability
141 performance, depending on the exposure class. Another study [22] collected the results of 1585 con-
142 crete mixes from different countries and concluded that it is possible to obtain a 20 MPa compressive
143 strength concrete with the minimum cement content (260 kg/m3). However, the literature shows no
144 consensus on minimum binder content requirements relative to the durability performance of concrete
145 [22, 23]. For example, a study [24] concluded that, apart from the strength class and water/cement ratio,
146 it may be unnecessary to impose a minimum cement content to reliably obtain an adequate durability
147 performance, as specified by standards [21]. Other studies [25-28] show that cement content can be
148 reduced without jeopardizing the durability performance. To date, the literature on this strategy is very
149 scarce [22, 24, 29-54].

150 The following sub-strategies are suggested to reduce the amount of binder in concrete.

151 3.1 Pozzolanic or hydraulic powders

152 Generally, most supplementary cementitious materials (SCMs) (§4) can be used in concrete to reduce the
153 binder content (by replacing a given amount of cement with SCMs) because they may significantly improve
154 some durability properties, except for carbonation in most cases. By lowering carbonation resistance, the
155 use of SCM is only recommended in concrete structures when not directly exposed to high CO2 contents
156 (e.g. foundation and underwater structures near chloride-enriched environments or watertight concrete -
157 §11.2.3), with unconventional reinforcement rebars (§11.1), or when involving great masses to reduce the
158 heat of hydration. Additionally, some attempts were made on low binder mortar. For example, Li et al. [55]
159 showed that the cement content of mortar can be reduced by 33% with an increase in strength of 33% by
160 using superplasticizer (SP) and ceramic polishing waste as addition [55]. This path can also be followed in
161 concrete [56]. Nonetheless, some studies [57-60] show that, even when carbonation resistance is involved
162 for XC3 and XC4 exposure classes, concrete with common cover depth can protect rebars for more than
163 50 years by using low or even high volume of SCMs.

164 3.2 Filler powders

165 The workability, stiffness and cohesiveness of concrete are significantly influenced by the volume of
166 paste [24, 53, 61]. Thus, low binder may negatively affect the mentioned properties of concrete and

9
167 indirectly influence other properties due to less-than-optimal compaction (e.g. in terms of strength and
168 porosity). One way to overcome this issue is by using (chemically non-active) fillers, namely marble waste
169 [29, 30, 62-65], limestone powder [37, 50, 66-68], quartz [69-72], dolomite [73-75], granite [76-79], cris-
170 tobalite [70, 72], nepheline syenite [70, 72, 80], wollastonite [70, 81-83], iron [76], soil [84], and talc -
171 hydrated magnesium silicate [31, 85]. However, studies on the effect of fillers in low binder concrete are
172 very limited [29-31] and mostly related to normal concrete with limestone filler [37, 50, 86] or self-com-
173 pacting concrete [29, 37].

174 Filler powders will also work as nucleation site-acting [69, 87-90]. For example, Penttala and Komonen
175 [38] obtained high mechanical (compressive and tensile) strength and durability performance (car-
176 bonation and capillary water absorption) concrete with a low binder amount (180 kg/m3 cement and
177 13 kg/m3 condensed silica fume -SF) and micro-filler (ground quartz). Another study of Tikkanen et al.
178 [39] showed that the strength of low binder concrete (cement type: CEM II/A-M(S-L)) can be increased
179 by adding mineral powder (limestone and quartz). This study did not focus on durability. However,
180 they showed that the Ca(OH)2 (the main contributor to carbonation resistance) content of concrete
181 mixes slightly decreases when mineral powder increases. This may happen because the filler, despite
182 its crystallinity and considerably smaller resulting porosity, reacted in the alkaline medium and con-
183 sumed Ca(OH)2 to create C-S-H. The same author [40] used the same type of cement and showed that,
184 by using mineral powders (limestone and quartz), 75 kg/m3 of cement can be removed without jeop-
185 ardizing the compressive strength. However, according to this study, the fine powder content should
186 not be higher than 550 kg/m3 because of pumpability requirements. Other fillers, e.g. quartz [69],
187 granite [77-79] and earth concrete [91], can be also used to promote nucleation sites.

188 3.3 Water to binder ratio (w/b) and dispersants

189 Generally, lowering the binder content of concrete by using this sub-strategy can be considered the
190 most promising solution in terms of sustainability, quality, and economy. Using the knowledge col-
191 lected from different studies [92-98], Figure 6 was drawn, and the results show that the quality of
192 cement paste essentially depends on the closeness of cement particles, rather than the binder content
193 or volume, and rate of hydration. Figure 6 shows that the porosity (linked to free water) of cement
194 paste with water to binder ratio (w/b) of 0.36 or lower is insignificant (almost non-porous materials)
195 because all the water content will be consumed by the cement particles. Nevertheless, more studies
196 must be made to confirm the previous assumption.

197 This can be concluded for concrete as well. Derived from the results of 140 concrete mixes, made with 140-

10
198 260 kg/m3 of cement, SCMs and different types of aggregates, sourced from 29 publications [99-128], Fig-
199 ure 7 shows that concrete with acceptable compressive strength can be produced with unconventionally
200 low binder content (grey background - Figure 7) when the w/b ratio is equal to or less than 0.40. This can
201 also be seen for low and high binder content (white background - Figure 7) that complies with EN 206-1
202 [21] standard (these are out of the scope of this section). Regarding the durability performance, by com-
203 paring the results of previous studies [53, 106, 129-137], it can be said that CO2 and chloride diffusion of
204 concrete exponentially decrease by lowering w/b to ≈ 0.36 (0.35-0.40) due to the smaller diameter of pores
205 that may not be easily penetrated by CO2 or any other agents. In other words, carbonation and chloride
206 ion penetration resistances are likely to be excellent in concrete with the mentioned w/b value. However,
207 further study needs to be performed to confirm this trend, especially when low binder content is used.

Unhydrated cement Cement gel Water gel Free water

1.0 0.09
0.21 0.21 0.20
0.8
Relative volume

0.27
0.30
0.6
0.67
0.4 0.79
0.64
0.50
0.2
0.13
0.0
0.30 0.36 0.42 0.60

w/c
208

209 Figure 6 - Hydration of cement paste with different w/b (Cement gel - water chemically reacted with cement particles; Wa-
210 ter gel - water physically linked with hydrated cement particles in a closed system although they have not reacted chemi-
211 cally yet and it significantly affects the rate of strength development; Free water - open porosity filled with water; further
212 details on the mentioned expressions are shown in [95, 138, 139])

213 However, the workability of these mixes needs to be such that the mixes are applicable on site. For that
214 purpose, water-reducing admixtures, fillers (to maintain volume ratio of aggregate to fine powder - §3.2)
215 and SCMs with spherical particles (e.g. FA) can be used. For example, some studies [47, 51] obtained a

11
216 reliable mechanical strength of low binder concrete by using SP. With the chemical admixtures available
217 on the market, it is possible to produce a workable concrete with w/b lower than 0.20 [94]. Additionally,
218 the EI of most chemical admixtures used in concrete is very small [140, 141], because of the small amounts
219 used relative to the bulk of concrete mix. Although chemical admixtures increase the total cost of concrete,
220 their cost can be offset by decreasing the cement content [142]. However, further study is needed to find
221 the optimum cement content by using chemical admixtures without affecting the total cost and perfor-
222 mance of concrete. Furthermore, for most concrete characteristics, the performance of SP in concrete with
223 blended cement is higher than that of the concrete with Portland cement [129, 143].

Strength vs w/c Strength vs binder content

Expon. (Lower bound) Expon. (Upper bound)

1.20 700

y = 1.3e-0.02x 600
1.00

500

Binder content (kg/m3)

0.80

400
W/b

0.60
300
260
0.40
200

0.20 y = 0.75e-0.02x 100

0.00 0
0 20 40 60

Compressive strength (MPa)

224

225 Figure 7 - Effect of w/b and binder content on compressive strength of concrete regardless of the type of aggregates and binder (cement
226 content = 140-260 kg/m3; No. of studies = 29; Workability S2-S3; Confidence interval of boundary lines = 95%; white background - concrete
227 mixes that comply with the binder content suggested by standard EN 206-1; grey background - concrete mixes with less binder content
228 than suggested by that standard)

229 Aïtcin et al. [94] showed that filler (non-reactive particles) will be fully encapsulated in a low w/b mix be-
230 cause the distance between cement particles is small. Thus, indirectly, the filler particles will significantly
231 contribute to the compressive strength of cement paste [93], and therefore the cement content can be
232 lowered. Thus, it can be said that, in regard to cement paste containing a filler, decreasing w/b can be more

12
233 effective than modifying the physical and chemical characteristics of cement.

234 Finally, according to the above discussion, low binder concrete with reliable technical performance, EI
235 and cost can be produced by lowering w/b to 0.40 (Figure 7), using SP, fillers and SCMs with spherical
236 particles, simultaneously. However, concrete with lower w/b must be even more carefully water-
237 cured. Otherwise, the uncontrolled development of autogenous and plastic shrinkage causes serious
238 early cracking that may compromise the durability performance of concrete structures.

239 3.4 Indirect reduction of the binder amount

240 In this sub-strategy, the binder content is decreased but none of the concrete’s technical characteris-
241 tics is jeopardized. In other words, the following solutions may not have been used in low binder con-
242 tent so far, but they are presented in this section as a clue to produce it: nanomaterials (§11.2.2.1),
243 binary-quaternary mixes (§4.4), stainless rebars (§11.1.1), barriers against the penetration of aggres-
244 sive agents (§11.2). The reasoning is, since they can improve the concrete’s characteristics, they can
245 be also used to offset the consequences of reducing the amount of cement.

246 Several studies [33, 44, 45, 50, 54] show that low binder concrete with acceptable technical charac-
247 teristics can be produced by considering particle packing models (e.g. Faury and Alfred mix design
248 models). For example, Carvalho [50] concluded that the durability and strength of concrete with 175
249 kg/m3 of cement designed by the particle packing models can be higher than concrete mixes designed
250 with traditional approaches using 250 kg/m3 cement content.

251 By considering all the above sub-strategies (section 3.1-3.4), low binder concrete may have low tech-
252 nical performance. As stated before, the best way to solve this issue is by lowering w/b (§3.2). How-
253 ever, this strategy may not work by itself. Thus, it is urgent to develop a new cement type for normal-
254 strength concrete that in general has better compatibility with most chemical admixtures, lower wa-
255 ter-demands, early strength-gain, lower heat-evolution compared with Ordinary Portland cement
256 (OPC), thus allowing a reduction of the binder content for the same final characteristics of concrete.
257 As suggested by other studies [94, 144-154], the ye'elimite-rich cement techniques (§4.5) can be con-
258 sidered a preliminary solution for the mentioned issues because the rheological problem (major issue
259 [94]) of low binder concrete can be controlled.

260 4 Reduce the environmental impacts and resources use of binders

261 Cement is the main contributor to energy consumption and greenhouse gas emissions in concrete [155,

13
262 156]. One strategy to decrease concrete’s EI is by replacing its cement with co-products and by-products
263 (without reducing the overall binder content). In this strategy, most of the researchers are focused on the
264 effect of SCMs on the technical performance of concrete. Apart from industrial waste ashes (§4.2), LCA
265 studies on other sub-strategies (§4.1 and §4.3-4.6) are very few. Most studies presume that the EI of con-
266 crete decreases by decreasing its cement content, by incorporating SCMs. However, this assumption may
267 not be correct when the service life of concrete is considered (examples regarding this matter are shown
268 in the first paragraph of section 11). Therefore, it is preferable to study simultaneously the technical per-
269 formance (e.g. mechanical and durability characteristics), EI/resources use (GWP, energy consumption,
270 abiotic depletion potential (ADP), eutrophication potential (EP), acidification potential (AP), ozone deple-
271 tion potential (ODP), photochemical ozone creation potential (POCP), renewable primary energy resources
272 (PE-Re), etc.), economy and toxicity of concrete. Then, it is possible to classify each product from a sustain-
273 ability point of view. In addition, the production process of some non-conventional materials involves sev-
274 eral steps, such as recovery, transportation and treatment that potentially present considerable EI. Thus,
275 all steps involved in concrete production from cradle to grave need to be considered.

276 4.1 Agricultural wastes and aquaculture farming as SCM

277 Generally, most of the agricultural wastes and aquaculture farming (AWAF) are burned as renewable
278 and sustainable energy resources, and they have remarkable potential as low-cost binders to be used
279 as SCMs in concrete. Contrary to industrial wastes (§4.2), LCA studies on concrete containing AWAF
280 ashes (AWAFA) as SCM are very limited. Regarding the technical performance, there is a consensus
281 (most references cited in §4.1) that the workability and drying shrinkage of concrete decrease with
282 increasing AWAFA content, and the opposite occurs for setting time. However, as shown in the fol-
283 lowing sub-sections (§4.1.1-4.1.10), other technical properties’ prevailing trends depend on the incor-
284 poration ratio and type of AWAFA. In addition, studies on the effect of AWAFA on the carbonation
285 performance of concrete are very limited.

286 Figure 8 presents the chemical composition of different types of AWAF such as rice husk ash (RHA - [157-
287 163]), corn cob ash (CCA - [164-166]), sugarcane bagasse ash (SBA - [108, 167-171]), wheat straw ash (WSA
288 - [172-175]), leaf ash [176-181], palm oil fuel ash (POFA - [182-186]), forest biomass bottom ash (FBBA -
289 [187, 188]), wood fly ash (WFA - [189-192]), olive waste ash (OWA - [193-196]), tobacco waste ash (TWA -
290 [197, 198]), elephant grass ash (EGA - [199, 200]) and mussel shell ash (MSA - [201-203]), sourced from 48
291 publications. The results show that there is a wide range in terms of the chemical composition of most
292 AWAF ashes. Thus, the performance of concrete containing the same type of AWAF ashes may differ be-
293 cause their characteristics dramatically change according to the combustion technique and genetic types

14
294 (e.g. white and black rise husks) of the AWAF [158, 187]. In other words, each region has different species
295 of animals (e.g. oyster shell) and plants that have unique chemical compositions. According to the litera-
296 ture, AWAF ashes can be used as an active binder when they are incinerated at about 1000 oC, because at
297 this temperature the quantity of amorphous particles increases [187, 204]. However, further studies need
298 to be done to confirm the quality of the AWAF ashes in terms of the burning technique.

100
content (%) 80
Al2O3+FeO3

60
40
20

299 0

100
content (%)

80
60
CaO

40
20
300 0

100

80
content (%)
SiO2

60

40

20

0
Forest biomass bottom…

Palm oil fuel ash

Wheat straw ash
Rise husk ash

Corn cob ash

Tobacco waste ash

Olive waste ash
Sugar cane bagasse ash

Mussel shell ash

Wood fly ash
Leaf ash
Elephant grass

301

302 Figure 8 - Chemical characteristics of rise husk ash, corn cob ash, sugar cane bagasse ash, wheat straw ash, leaf ash, palm oil fuel ash,
303 forest biomass bottom ash, wood fly ash, olive waste ash, tobacco waste ash, elephant grass and mussel shell ash [108, 157-200]

304 4.1.1 Rice husk ash

305 Relatively to other AWAFA, RHA is the most common material studied in the literature. Well burned
306 rice husk (RH) may contain a high amount of amorphous silica. However, its quantity significantly de-
307 pends on the type of RH, i.e. black or white [158]. Apart from workability [161], most of the concrete
308 technical performances, i.e. strength [158-160], carbonation [205], shrinkage [160], porosity [160,
309 206], water absorption [206] and chloride ion penetration [159], improve or remain similar to those
310 of conventional concrete when cement is replaced with up to 20% of RHA [157-163].

15
311 4.1.2 Palm oil fuel ash

312 After RHA, POFA is the second most studied AWAF. The literature suggests that POFA can be used in high-
313 strength concrete due to its high ratio of ultrafine particles [184, 207-211]. Generally, it is suggested that
314 POFA can be effectively used as SCM to replace up to 20% of cement in concrete [184, 185, 210, 212].

315 4.1.3 Corn cob ash

316 According to the literature, the optimum incorporation ratio of CCA depends on the type of CBM (e.g.
317 paste and concrete). Although some studies [166, 213, 214] have been concluded that the paste con-
318 taining up to 15% of CCA complies with NIS 439:2000, ASTM C 150:1994 and BS 12:1991 requirements
319 [166, 213, 214], there is a consensus in the literature that cement of concrete should not be replaced
320 with more than 10% of CCA [164, 165, 215, 216].

321 4.1.4 Sugarcane bagasse ash

322 Different replacement levels (5-25%) are given by the literature as optimum values to substitute cement
323 with SBA in concrete [217-222]. Cordeiro et al. [223] concluded that SBA must be burned at least at 600
o
324 C for 3 hours to obtain amorphous and low carbon content precursor. Nevertheless, this temperature
325 may not be enough to degrade the entire carbon-containing phases. The optimum incorporation ratio
326 of SBA depends on the target properties of concrete, i.e. 10% [167], 15% [219], 20% [224], 5-20% [217,
327 218, 225], 25-30% [167, 219] and 25% [219] to obtain improvements in water absorption, sorptivity,
328 strength, chloride penetration, chloride penetration and soundness, respectively.

329 4.1.5 Straw ash

330 Studies on the effect of straw ash as a partial substitute for cement in concrete are very limited and
331 mostly related to WSA. This is maybe related to the fact that the results are not promising relatively to
332 other AWAF [173, 226, 227]. However, it is mostly used for other applications [172, 174, 175, 228, 229].
333 There are also a few studies on the effect of the use of rice straw ash [230] and rape-plant straw ash
334 [231] on the technical performance of concrete and mortars [232]. Other straw ashes, made with barley
335 [233], corn [234], and rape [234] straws, have similar chemical compositions to WSA.

336 4.1.6 Leaf ashes

337 Amorphous and pozzolanic ash can be obtained by incinerating banana [235, 236] and bamboo [177,
338 179, 237] leaves. It was concluded that the activity of bamboo leaf ash (BLA) is greater than that of RHA
339 and SBA [180]. The results show that cement can be replaced with up to 15% [178] and 20% [235, 238]

16
340 of each BLA and banana leaf ash, respectively, for a compromise between the durability and strength
341 performances. Nevertheless, a study produced low binder content concrete with a high w/b ratio and
342 showed that the strength decreases with increasing BLA content [239]. Apart from the mentioned ashes,
343 there are other leaf ashes, used only in pastes and mortars [176, 181].

344 4.1.7 Forest biomass bottom ashes

345 Forests must be isolated and divided in several zones to prevent uncontrollable fires. Normally, the isolated
346 zones must be cleaned of all the grass, wood, straw, leaves, etc. For sustainability reasons, these forest
347 residues can be used to obtain renewable energy and use their ash for construction purposes. Accordingly,
348 these ashes may have significant ranges in terms of chemical and physical properties, depending on the
349 source of biomass. Previous studies [187, 240] showed that strength may slightly improve with the incor-
350 poration of 10-15% FBBA as cement substitution, especially after 90 days. Several studies on the effect of
351 forest residues ashes on mortar have been made [187, 188, 240, 241]. However, this path has not been
352 followed for concrete.

353 4.1.8 Wood ashes

354 Although wastes from forests (section 4.1.7) contain a variety (contaminated) of materials, quite often
355 their characteristics may not be that different from those of wood ashes. A couple of studies [242,
356 243] showed that the majority of wood ashes (WA) have lower SIO2+Al2O+Fe2O3 and higher CaO con-
357 tent than those of coal ashes. This helps concrete to develop more C-S-H. However, the amount of
358 loss on ignition (LOI) in WA is significantly higher than that of the coal ashes, which negatively affects
359 the performance of concrete. Most of the studies show that the mechanical performance of concrete
360 decreased with increasing incorporation ratio of WA [244-247]. In terms of durability, namely chloride
361 ion penetration, there is no consensus in the literature, but some studies showed that it may increase
362 durability by being incorporated with other SCM [242]. WA is also harmful in terms of carbonation
363 [242] and water absorption [244], but it may decrease the carbonation rate with FA because of the
364 synergetic behaviour of the two materials [248]. In addition, despite several attempts [242, 244-247,
365 249-251] to understand the effect of WA on concrete, Magi et al. [250] stated that there is no detailed
366 study on the effect of WA on high-strength concrete. Furthermore, attempts to treat WA before using
367 it as SBM are very limited [252].

368 The bark ashes of most trees (balsam [253], beech [253], pine [254], birch [253], elm [253], eucalyptus
369 [254], hemlock [253], maple [253], poplar [253], spruce [253], and tamarack [253]) contain a signifi-
370 cant amount of CaO (43-68%) that is very close to that of ordinary Portland cement. However, studies

17
371 on their effect on concrete have not been made. For example, although the amount of CaO in cement
372 and the mentioned materials may be the same, it does not necessarily have the same potential in
373 terms of reactivity. In fact, their potential depends on the ratio of amorphous particles.

374 4.1.9 Other agriculture-farming wastes

375 There are also few attempts to use other farming wastes ashes such as those from the olive [194, 195,
376 255], tobacco [197], elephant grass [199], banana [256], sisal [257] and ripe plantain peels [258] sec-
377 tors as SCMs in concrete. According to the mentioned studies, the performance of farming waste
378 ashes depends on their exposure to heat that directly affects the amount of amorphous particles.

379 4.1.10 Shell wastes

380 Most of the shells are used as partial replacement of natural aggregates in concrete (§5.2). However, some
381 attempts have been made to show the effect of oyster shell ash as partial replacement of cement on the
382 technical performance of mortar [201, 202], as well as that of mussel shell ash [201, 202], periwinkle shell
383 ash [259, 260], cockle shell ash [261] and eggshell [262] on cement pastes, mortars and concrete. According
384 to the mentioned studies, the shell ashes generally decrease strength, drying shrinkage and thermal con-
385 ductivity, increase setting time, and improve resistance to magnesium-sulphate attack.

386 4.2 Industrial wastes as SCM

387 Contrary to AWAF, there are many studies on the effect of industrial waste ashes as substitutes of
388 cement on the cost, EI and quality of concrete. However, further study on the majority of these ma-
389 terials is still needed due to their discrepant chemical composition. Using the ternary phase diagram,
390 Figure 9 is drawn, presenting the chemical composition of different types of binders, sourced from 81
391 publications [108, 157-196, 199, 200, 263-300]. The results show that the chemical composition of
392 industrials wastes relatively to AWA (§4.1) are more discrepant and significantly depends on the type
393 and source of the materials. It is important to mention that the data given in Figure 9, namely the
394 amount of CaO, Al2O3 and SiO2 given for each material (e.g. CFA and GGBS), cannot be directly com-
395 pared with the same amount in cement because the amount of amorphous particles in these materials
396 is different from that in cement.

397 4.2.1 Coal fly ash

398 According to the American [301] and Canadian [302] standards, which are comparable to European stand-
399 ard [303], FA is classified as high (type C) and low (type F) CaO content. Relatively to other industrials

18
400 wastes, type F coal FA is the most common material used in the literature regarding technical perfor-
401 mance [104-106, 108, 111, 116, 118, 125, 126, 130, 304-348], LCA [9, 129, 140, 326, 341, 349-353], cost
402 [141, 155, 354], and toxicity [155, 355-363]. Nevertheless, studies on the service life and toxicity of con-
403 crete containing a high volume of FA are still very limited. According to most of the previous studies [104-
404 106, 108, 111, 116, 118, 125, 126, 130, 305-348], the technical properties of concrete may worsen when
405 a high volume of cement is replaced with FA type F. Some researchers overcame this issue by replacing a
406 given amount of cement with FA and adding extra FA as an addition [41, 125, 364].

407

408 Figure 9 - CaO-SiO2-Al2O3 ternary phase diagram of different binders. AWA = agricultural wastes (rise husk ash, corn cob
409 ash, sugarcane bagasse ash, straw ash, palm oil fuel ash, forest biomass bottom ash, wood ash), BF = Brick feedstock, BF =
410 brick feedstock, CBA = coal bottom ash, CL = clay, CS = copper slag, FA = coal fly ash, FG = flat glass, GGBS = ground granu-
411 lated blast furnace slag, HL = hydraulic lime, MIBA = municipal solid waste incinerator bottom ash, NP = natural pozzolan,
412 PC = Portland cement, QL = quick lime, SF = silica fume, SH = shale, SLG = soda lime glass. Texts with red and black colours
413 are average value and range values, respectively. C = CaO, S = SiO2, A = Al2O3 (grey texts). AFt = ettringite, AFm = monosul-
414 phate, C-S-H = Calcium-Silicate-Hydrate (blue texts). CS, C2S, C3S, lime are reactive to CO2. Data obtained from [108, 157-
415 196, 199, 200, 263-300]

19
416 4.2.2 Coal bottom ash

417 CBA is mainly recommended to be used in concrete as a partial replacement of sand because it has
418 less active SiO2 content compared to FA and its particles are porous, irregular and angular, and have
419 a rough surface texture [267, 365-368]. However, some studies show that it can also work as a poten-
420 tial SCM after proper grinding [369]. Most of the previous studies are focused on the effect of CBA, as
421 cement replacement, on concrete strength [267, 370-377], and a few studies focused on durability
422 [370, 378, 379], toxicity [362], EI [380-383] and cost [383]. Based on the mechanical strength, CBA is
423 recommended to be used at up to 10% of cement’s weight [370-372].

424 4.2.3 Industrial slags

425 Industrial slags are another by-product remaining after an intended metal smelts from its raw ore. To
426 produce more sustainable concrete, cement has been substituted with ground granulated blast furnace
427 slag, i.e. lead slag [384], copper slag [385-387], nickel slag [388], and iron slags [389, 390]. Due to their
428 high density, reactivity and/or pozzolanicity, most of the mentioned slags were recommended to be
429 used as aggregates for radiation shielding concrete [391-394]. However, due to their chemical composi-
430 tion (Figure 9), ground granulated blast furnace slag (a by-product of iron and steel-making) is also stud-
431 ied as SCM in terms of quality [395-397] and EI [353, 398, 399]. However, this solution significantly in-
432 creases the dead loads of the concrete structure.

433 4.2.4 Silica fume (SF)

434 SF has been successfully used for many applications [309, 397, 400-407], and it may act as a healing
435 agent, filler and SCM in concrete [131, 309, 316, 318, 330, 408-413]. SF significantly increases strength,
436 pozzolanic activity [403, 405, 406], durability and impact resistance [309, 400-402, 414] of concrete
437 due to its multi-range macro-particles and chemical composition. Existing standards such as European
438 standard [415] already have the recommended amount of silica fume that cement may have when
439 using conventional materials (e.g. natural aggregate). Regarding non-conventional materials such as
440 recycled aggregate and steel fibres, 10%-14% of SF considered as an optimum [309, 400, 402]. Never-
441 theless, SF may decrease workability [416] and long-term compressive strength [417] and it is not
442 easily dispersed in concrete. In addition, SF may not be effective in terms of creep [418] and corrosion
443 resistance in marine environment [419].

444 4.2.5 Other artificial pozzolans

445 Artificial pozzolans can be classified as industrial by-products (most of SCM in §4.1-4.3) and burned

20
446 materials, namely (i) calcined clays [397, 420-427], (ii) ceramic residues [55, 56, 428-431], (iii) sedi-
447 mentary rocks containing clay minerals [432-434] and (iv) burned bauxites [435, 436].

448 Natural calcined clay such as kaolinite [426, 437, 438], montmorillonite [437, 438], and muscovite/illite
449 [437, 438] can be used as SCM [426]. However, the most common one is metakaolin [397, 421-425],
450 which is derived from calcined kaolin clay. Their performance significantly depends on the calcined
451 temperature (600-850 °C for 1-12 h) [439]. The use of metakaolin in the construction sector is still far
452 behind that of the other SCMs because of its price (3-4 times higher price than that of cement [434]).

453 Ceramic residues [55, 428, 429] or ceramic polishing waste [56, 430, 431] are other active pozzolans
454 and they are considered as the illite group [434], used for the production of red-ceramics. After milling,
455 they can be used as a partial replacement of cement [55, 56, 428-431]. However, studies in this path
456 are still very limited and the ceramic residues powder is not widely available [434].

457 Sedimentary rocks contain clay minerals, also termed calcined shale [432, 440, 441] and claystone
458 [434]. Although they may be an alternative solution to the other two artificial pozzolans [434], due to
459 their lower price and availability, studies on these materials are still very scarce.

460 In the aluminium industry, sedimentary rock (bauxite) with a relatively high Al content is burned. As a
461 result, a significant amount of hazardous waste (red mud) is generated (this can also be included in
462 §4.2.3). This bauxite residue is considered as an effective SCM to be used as partial replacement of
463 cement in concrete [435, 436].

464 4.2.6 Natural pozzolans

465 Natural pozzolans are sourced from (i) volcanic tuffs/zeolites [442, 443], (ii) siliceous such as opal and
466 diatomaceous earth [433, 434, 444-446], and (iii) volcanic glasses such as volcanic ashes [447-449],
467 pumice and pumicite [450, 451]. Most of the conclusions drawn for artificial pozzolans can be apply
468 to concrete containing natural pozzolans, except the fact that it costs less [443, 447]. In other words,
469 the cost of concrete can significantly decrease by increasing the incorporation ratio of natural pozzo-
470 lans because they do not need to be burnt.

471 4.3 Municipal wastes as SCM

472 4.3.1 Glass powder

473 Glass is an amorphous and non-crystalline material. It has been used as partial replacement of aggre-

21
474 gate in concrete [452-459] and in other products such as fired-clay bricks [460], alkali-activated mate-
475 rials [461, 462], glass-reinforced panels [463], structural repair mortar [464], ultra-lightweight fibre-
476 reinforced concrete [465], micro filler for concrete [452, 454], lightweight aggregates [466] and con-
477 crete blocks [459]. However, sometimes the results are not satisfactory when waste glass is used as
478 aggregates in concrete due to a destructive reaction between silica in waste glass aggregate and alkalis
479 in Portland cement that form silica gel (the main contributor to expansion) and micro-cracks generate
480 around the reactive aggregates [457]. Nevertheless, several studies concluded that very fine glass
481 powder as a partial replacement of cement in concrete may have sufficient pozzolanic properties and
482 no detectable deleterious action from alkali-silica reaction and they reported several replacement ra-
483 tios (40% [467], 20% [468], 15% [469], 10% [470]) as an optimum. Additionally, glass can be considered
484 as industrial (e.g. from car manufacturers) and municipal (flat glass sourced from households) waste.

485 4.3.2 Sludge ashes

486 Sludges are semi-solid slurries mostly produced from drinking water and wastewater treatment
487 plants. Since dried sludge has similar heat value (calorific) to that of brown coal [471-473], its incin-
488 eration has become more attractive lately. For sustainability reasons, the ashes resulting from burning
489 these sludges, such as sewage sludge ash (SSA) [474-479] and sludge wastewater sludge ash [480],
490 can be used as a partial replacement of cement in concrete. Generally, only low contents of SSA can
491 be used [481]. For higher quantities, treatment is required to extract phosphorus [481, 482]. Gener-
492 ally, they can be used as aggregates [483, 484], as binder [479, 485], in blocks [476, 486], in lightweight
493 aggregate concrete [487, 488], and in aerated/foamed concrete [489].

494 Apart from the above sludges, paper sludge [490-493], granite waste sludge [494, 495], galvanic sludge
495 [496], glass waste sludge [497, 498], paint sludge [499], and contaminated arsenic sludge [500] are
496 also used, after burning or drying, in pastes, mortars and concrete.

497 4.3.3 Municipal solid waste incineration ashes (MIBA)

498 In terms of chemical composition, MIBA can be divided in “pozzolanic regions” and “latent hydraulic”
499 [263], depending on the combustion temperature and the source of the solid waste. Most studies are
500 focused on the effect of MIBA on the compressive strength [501-505] and leachability [502, 505-507]
501 of concrete. Generally, MIBA are detrimental to the strength of concrete due to the reaction between
502 cement and aluminium of MIBA [263, 505]. Regarding municipal solid waste incineration fly ash, high
503 chloride ions content is the main detrimental aspect to its potential use [360, 507-511].

22
504 4.4 Binary, ternary and quaternary SCM mixes

505 So far, there is no systematic review on the effect of binary, ternary and quaternary SCMs (BTQ-SCM)
506 on the performance of concrete, specifically for incorporation ratios of SCM higher than the standard
507 limit [415]. Additionally, consensus on the negative and positive effect of this path cannot be reached
508 [159, 397, 512-516]. Nevertheless, according to the results of most studies [159, 397, 513-515], the
509 synergetic behaviour of BTQ-SCM with normal particle size (> 100 nm) and specific surface area (<
510 10,000 m2/kg) [517] may not be significant. However, promising results are shown by using one or two
511 SCMs with normal particle size and a small quantity of nano SCM particles, such as nano SiO 2 [309,
512 518-520], nano CaCO3 [378, 521, 522], nano TiO2 [523-526], nano Fe2O3 [527-529], nano Al2O3 [527,
513 530], nano ZnO [531, 532], and nano clay [533, 534].

514 4.5 Alternatives to Portland cement clinker

515 Another solution to promote sustainability, instead of replacing cement with SCMs, is by producing
516 alternative cement clinker such as ye'elimite-rich cements - binders based on phosphates [535-537], ,
517 magnesium-based cements [538, 539], thermal activated low-carbon recycled cement [540], binders
518 by activating of liberated concrete fines (recycled concrete fines are activated through a thermal treat-
519 ment method) [541], and binders based on reactive calcium silicates produced by hydrothermal pro-
520 cessing techniques [542, 543].

521 Generally, Ye'elimite-rich cements can be divided in two main groups (i) low belite (calcium sulphoalu-
522 minate cements - CSA) such as reactive belite-rich Portland cement clinkers [144-148], and (ii) high
523 belite such as belite-ye'elimite-ferrite binders [144, 146, 149], belite-alite-ye'elimite binder [149-152],
524 and belite-ye'elimite-ternesite binder [149, 153, 154]. Generally, these cements require a lower tem-
525 perature, but their performance is worse than that of OPC.

526 However, studies regarding these new cement clinkers are very scarce due to the cost barriers [146]
527 and the fact that it is complicated to simulate it in laboratory conditions such needed operations as
528 filling a “rotary clinker kiln” with the raw materials used to make these cements.

529 4.6 Activation techniques and geopolymer

530 One way to promote sustainability is by utilizing co-products or by-products as partial replacements of
531 cement. However, their incorporation ratios are limited because, after a given ratio (high volume), further
532 hydration products in the paste may not be produced. To overcome this issue, alkaline activator (e.g.

23
533 NaOH, KOH, and Na2SiO3) can be used. Thus, alkali activation techniques can be considered an alternative
534 process to partial replacement of cement with SCMs. Materials that are rich in amorphous Al2O3 and SiO2
535 can be used as a precursor, such as:

536 i. AWAF: RHA [544, 545], POFA [546-549], CCA [550, 551], SBA [552], straw ash [550, 553], FBBA [554],
537 WA [555, 556], other agriculture-farming wastes (e.g. alfalfa steam ash, cotton gin ash, com stalk ash
538 and switch grass ash - [550, 557, 558]), and shell wastes [559, 560];

539 ii. Industrial waste ashes: FA [561-568], CBA [569], industrials slags [546, 563, 570-575], SF [576-583],
540 artificial pozzolans (calcined clays [575, 584-586], ceramic residues [587, 588], sedimentary rocks con-
541 taining clay minerals and burned bauxites [589-591]), natural pozzolans (volcanic tuffs/zeolites [442,
542 443], siliceous such as opal and diatomaceous earth [433, 434, 444-446], and volcanic glasses such as
543 volcanic ashes [447-449, 592, 593], pumice and pumicite [594, 595], mine mud waste [596-599]);

544 iii. Municipal waste ashes: glass powder [461, 600-605], sludge ashes [491, 493, 606-608], MIBA [609-
545 631], and municipal solid waste incinerator fly ash (MIFA) [507, 632-639].

546 Alkali-activated materials (AAM’s) can be also produced with blended SCMs. For example, GGBS-SBA
547 [552], biomass FA-metakaolin [191], RHA-GGBS [574], FA-metakaolin [640, 641], POFA-FA [546], FA-
548 RHA [642], FA- SF [576, 578, 580-582], and FA-slag [643-647] blends have been used. FA with spherical
549 particles to control the fresh properties is used as SCM to produce AAM [546, 640-645, 647-649]. In
550 other words, most AAM studies are related with industrials wastes because concrete with different
551 mechanical performance (e.g. 55-60 MPa [642], 20-60 MPa [644], 30-62 MPa [647], 20-60 MPa [646],
552 20-50 MPa [645], 20-70 MPa [648]) can be obtained from their use for a regular curing temperature
553 (20-23 °C). Relatively to industrial waste ashes, studies on AAM containing agricultural and municipal
554 waste ashes are still very few. Perhaps this happens because the results are not promising when agri-
555 cultural and municipal waste ashes are used in AAM alone [544, 610-631, 650-654]. One way to boost
556 the performance of AAM is by blending one SCM with nanoparticles, especially nanosilica [519, 577,
557 655-662] or ultrafine slag (alccofine - [663-666]), or low quantity of cement [642, 644, 667-672].

558 5 Reduce the environmental impacts and resources use of aggregates

559 Replacing virgin aggregates [673] with non-conventional aggregates is another strategy that can be
560 used to promote sustainability. However, relatively to other strategies (e.g. reduce the EI of binder,
561 §4), the EI of concrete can only slightly decrease (up to 10% [101, 141, 341, 674], mostly depending

24
562 on transportation scenario [350, 675, 676]) or slightly increase [7, 677]. For that purpose, many spec-
563 ifications, e.g. from Portugal [678], UK [679-681], Austria [682], Japan [683-685], Denmark [686], Brazil
564 [687], Holland [688-690], Switzerland [691], USA [692], Germany [693], France [694], Spain [695], China
565 [696], Australia [697], and others [698] have been developed based on the technical properties of re-
566 cycled aggregates, i.e. components, water absorption, density and maximum incorporation level in
567 concrete and other construction materials. However, the specifications have not defined any limita-
568 tions in terms of LCA. This gap is directly associated with the lack of joint investigation/data in terms
569 of LCA and technical properties of recycled aggregates concrete.

570 5.1 Construction and demolition waste

571 5.1.1 Recycled concrete aggregate

572 Concrete can be found in most recycled aggregates due to fact that it is the most consumed material
573 in structural applications. It can be separated from other construction and demolition waste (CDW)
574 materials and re-used in concrete. Generally, the effect of recycled concrete aggregate (RCA) on the
575 technical properties of concrete depends on its replacement level [699-702], water absorption [102,
576 104, 105, 110, 135, 702-740], moisture content [702, 741], size [101, 143, 700, 741-747], shape [700,
577 741, 747], density [102, 104, 105, 110, 135, 702-741], recycling procedure [741, 746, 748-750], and
578 quality of the original material [737, 741, 750-754], and on the composition of the resulting concrete,
579 i.e. water to cement ratio [409, 721, 741, 743, 755-758], chemical admixtures [117, 741, 759-761],
580 type of binders [101, 103, 104, 106-108, 111, 113, 116, 118, 121, 126, 130, 140, 143, 305, 337, 339,
581 341, 720, 741, 746, 762-767], and environmental conditions [741, 768, 769].

582 There is a wide range in the characteristics of RCA due to the quality of the original material [770] and
583 the size of the aggregates [101, 771]. For example, the water absorption, saturated surface-dry (SSD),
584 particle oven-dried, apparent, and loose bulk density of fine RCA are 3.5-13%, 2161-2929 kg/m3, 1913-
585 2620 kg/m3, 2410-2600 kg/m3 and 1344 kg/m3, respectively [135, 719, 722-740]. In addition, the water
586 absorption, loose bulk density and particle oven-dried density of coarse RCA are 2.8-6.8%, 1230-1600
587 kg/m3 and 2140-2760 kg/m3, respectively [102, 104, 105, 110, 703-721].

588 In general, fine RCA is more detrimental to concrete than coarse RCA due to its high mortar content that
589 increases its water absorption. In terms of strength, some studies mentioned that 20-30% incorporation of
590 RCA may have a minor impact on concrete [744, 772]. Nevertheless, the effect of RCA depends on the
591 target strength of concrete. For example, by sorting the results of the following studies based on their
592 target strength: 20-30 MPa [701, 719, 773, 774], 30-40 MPa [709, 713, 733, 757, 775-780], 40-50 MPa [134,

25
593 703, 704, 715, 728, 739, 778, 781, 782], 50-60 MPa [704, 715, 744, 783, 784], 60-70 MPa [712, 736, 744,
594 783-785], and 70-80 MPa [736, 783, 784], it can be said that the strength of high-strength concrete sharply
595 reduced with increasing RCA replacement (failure will occur in the weaker old adhered mortar of RCA rel-
596 ative to the cement paste of conventional concrete). This may not occur for low strength concrete (at least
597 up to 30% incorporation) because the ultimate strength of low-strength concrete depends mostly on its
598 cement paste characteristics. In addition, most properties of concrete containing RCA have been studied,
599 i.e. fresh properties [119, 134, 699, 786], tensile strength [744, 781, 787], modulus of elasticity [723, 727,
600 782], carbonation [788-790], chloride penetration resistance [756, 791], water absorption [119, 756, 792-
601 795], shrinkage [119, 727, 782, 796], UPV [781, 782], creep [796, 797], LCA [5, 7, 12, 129, 350, 744, 798-
602 802], cost [141, 142, 803, 804], and toxicity [805, 806]. However, studies on the combined effects on tech-
603 nical performance, LCA and cost are very few.

604 5.1.2 Recycled Masonry Aggregate (RMA)

605 The composition of recycled masonry aggregates (RMA) is identified to be a minimum of 90%, by mass,
606 of mortar and burnt clay materials such as ceramic roofing tiles and shingles, ceramic bricks, light-
607 weight concrete blocks, sand-lime bricks, and blast-furnace slag bricks and blocks [741, 807]. Accord-
608 ing to the results of 787 concrete mixes collected in [702], after RCA, RMA is the second most suitable
609 type of CDW aggregates to be used in concrete. In other words, for a given incorporation ratio, RMA
610 is more detrimental than RCA in concrete because of the former’s lower density, higher water absorp-
611 tion, and higher Los Angeles abrasion loss [741, 808]. Based on the results of these studies, the 95%
612 quantile highest strength loss of concrete mixes made with 100% of coarse RMA is 50%. The suitability
613 of RMA in concrete can be also confirmed by other technical performances such as tensile strength
614 [809-814], modulus of elasticity [809, 815], carbonation [808, 816], chloride penetration [808, 811,
615 817, 818], water absorption [808, 811, 817], shrinkage [819] and creep [820]. However, there are no
616 detailed studies on life-cycle environmental and economic assessment.

617 5.1.3 Contaminated construction and demolition waste

618 CDW that contains high amount of different contaminations (e.g. wood, glass, asphalt and plastics)
619 can be used as aggregates in concrete [821, 822]. However, the literature has limited detail on the
620 composition and origin of this type of aggregates [741, 823]. A revision of Silva et al. [741] considered
621 results of 116 studies and showed that, for a 95% confidence interval, the average (lower and higher
622 bounds) oven-dried density, saturated surface-dry density, and water absorption are 2280 kg/m3
623 (2241-2318 kg/m3), 2399 kg/m3 (2366-2431 kg/m3), 5% (2-32%) for coarse mixed construction and
624 demolition recycled aggregates (CDRA), and 2207 kg/m3 (2161-2253 kg/m3), 2399 kg/m3 (2364-2433

26
625 kg/m3), 8% (4-50 %) for fine CDRA, respectively.

626 Similar factors mentioned in section 3.2 may affect the influence of mixed CDRA on the technical perfor-
627 mance of concrete. Apart from these factors, the chemical composition of CDRA, namely sulphate [746,
628 824, 825], chloride [826], and alkali contents [100, 772, 826], may significantly compromise the perfor-
629 mance of concrete. For example, most specifications are limited and concerned about the maximum sul-
630 phate content (0.8% [678, 693, 827] or 1.0% [687, 691, 695, 696, 698]). Furthermore, for similar mix com-
631 positions, relatively to uncontaminated CDW aggregates, there is a big scatter between the performance
632 of concrete mixes made with mixed CDRA [828-834]. This can be mainly explained by the percentage of
633 contaminated materials [835-838], such as gypsum (main responsible for sulphate expansion [807, 839])
634 and reactive silica [100, 772, 826]. The review conducted by Silva et al. [702] based on the results of 787
635 concrete mixes containing different types of CDW aggregates did not recommend using mixed CDRA in
636 concrete unless they are adequately tested for their composition and properties before use.

637 5.1.4 Mixed Recycled Aggregate (MRA)

638 In spite of the conclusions of the previous section (§5.1.3), mixed CDRA can still have benefits by sep-
639 arating concrete and masonry particles and using this mixture as mixed recycled aggregates (MRA).
640 Thus, this type of aggregate can be considered as intermediate between RCA (§5.1.1) and RMA
641 (§5.1.2). Recently, a jigging technique was suggested to separate brick/concrete particles in mixed
642 CDRA [837, 840, 841] but studies on this separation technique are very limited. Some specifications
643 [78, 86] identified the composition of this type of aggregates (less than 90% of natural aggregates and
644 Portland cement-based fragments). Thus, it may include other CDW common materials such as light-
645 weight concrete and ceramic [741, 842-845]. According to the statistical analysis made in the study of
646 Silva et al. [702], the 95% quantile maximum strength loss of concrete mixes made with 100% of coarse
647 MRA is 60%. Other technical performances decay with the use of MRA [100, 808, 813, 846-850]. How-
648 ever, MRA still can be recommended for construction materials, especially for low-strength concrete.

649 5.2 Agricultural wastes and aquaculture farming as aggregates

650 As shown in §4.1, cement in concrete can be replaced with many types of AWAF ashes. Due to dump-
651 ing problem of agricultural wastes and global demand to aggregates (due to rapid urbanization), many
652 agro wastes can also be used in concrete as a partial replacement of aggregates, especially as a fine
653 aggregate. Apart from sustainability reasons, the purpose of this strategy is to produce lightweight
654 and low thermal conductivity concrete [851-854]. On this path, most of the studies are focused on the

27
655 technical properties of concrete containing bottom AWAF (as raw material and ash) as a partial re-
656 placement of sand such as SBA [855, 856], groundnut shell [857, 858], sawdust [859, 860], wild giant
657 reed ash [861], wheat straw [862, 863], WA [864], rice husk/ash [865-867], cork [868, 869], tobacco
658 waste [870], CCA [863, 871], leather [872], palm tree shell [852, 873-882], plane leaf ashes [863] and
659 olive husk [883], sunflower [884], seashell (e.g. oyster [885-889], mussel [888, 890], cockle [888, 891],
660 scallop [888, 892], and periwinkle [888, 893, 894]). Most of the studies on this path are related to palm
661 tree shells [852, 873-882]. Additionally, only compressive strength has been studied in detail.

662 5.3 Industrial wastes as aggregates

663 Similarly to AWAF, industrial wastes can also be used as fine natural aggregate replacement in con-
664 crete. De Brito and Saikia [895] and Rashad [853] made extensive literature reviews about this strat-
665 egy. The results show that most of the studies are focused on the effect of artificial pozzolan wastes
666 (§5.1.2-5.1.4) as sand replacement in concrete, followed by natural pozzolans (e.g. volcanic tuffs/zeo-
667 lites [896-899], siliceous [900, 901], and volcanic glasses [902-905]), FA [906-914], CBA [271, 915-921],
668 iron and steel slags such as blast furnace slag (e.g. ground blast furnace slag [922-925] and air-cooled
669 blast furnace slag [926, 927]) and steelmaking slag (e.g. converter slag [928] and electric arc furnace
670 slag [929-935]), SF [936-938], plastic waste (§5.5), rubber waste (§5.5), and then distantly followed by
671 non-ferrous slags (e.g. copper slag [934, 939-943], lead and zinc slag [944, 945]). These types of aggre-
672 gates can reduce the cost and EI and enhance several durability properties of concrete. However,
673 widespread reliable data are missing for the use of these aggregates in concrete.

674 5.4 Municipal wastes as aggregates

675 Similarly to industrial wastes, municipal wastes as a raw material and ashes are used in concrete as a
676 partial replacement of natural aggregates, in the shape of glass (§5.5), MIBA [263, 946-952], SSA [476,
677 482-484, 953, 954], wastewater sludge ash [954-956], paper sludge [490], and granite waste sludge
678 [957-959]. Most of the studies related to concrete containing municipal waste aggregates are focused
679 on compressive strength.

680 5.5 Insulating aggregates

681 Normally, non-conventional aggregates are used to consume less virgin aggregates. However, some
682 of them (e.g. plastic, rubber and lightweight aggregates) can be used for other sustainability purposes,
683 namely to decrease the thermal conductivity of concrete (see section 13.2). They can be used in dif-
684 ferent applications of concrete. This strategy can also be identified as industrial waste (§5.3).

28
685 The fast growth of the global tires market and their short service life are another serious environmental
686 issue (3 billion units in 2019 with forecast 7% growth rate [960]). One way to promote sustainability is by
687 using tire waste aggregate in concrete (rubberized concrete). Most of the technical properties of rubber-
688 ized concrete have been studied, such as fresh properties [961-963], shrinkage [961, 964-966], mechanical
689 strength [961, 962, 966-968], chloride ion penetration [963, 964, 969], freeze/thaw resistance [961], fire
690 resistance [961, 970], thermal insulation [961] corrosion resistance [961], resistance to aggressive environ-
691 mental [961, 971], carbonation [964, 972], sound absorption [961, 973], water permeability [962, 964, 969,
692 973], and density [962, 968]. According to the cited studies, rubber content in concrete must be limited to
693 up to 30% in order to guarantee an acceptable level of mechanical performance. The results show that tire
694 waste aggregate enhances the energy absorption ability, ductility, and electrical resistivity of concrete [961,
695 966, 972, 974, 975]. Contrary to other types of recycled aggregates, fine tire waste aggregate is less detri-
696 mental than coarse particles [974, 975].

697 According to the first review study made in [976], the concept of using plastic waste as a partial replace-
698 ment of natural aggregates in concrete is relatively new. Nowadays, many studies are made on this path
699 [977-985] especially because of the amount of plastic wastes in the industry (e.g. electronic plastics
700 waste). Most of the studies suggested using plastic waste aggregate in the production of non-structural
701 concrete or temporary structures. Nevertheless, by using different forms of waste plastic (e.g. waste
702 plastic flakes [986, 987], polyvinyl chloride pipe [988], polyethylene terephthalate particles [989-991],
703 high-density polyethylene waste [992], shredded fibres of polythene bags [993], PET bottle fibres [994],
704 and PET waste [995]), the performance of concrete increased, especially when used as a fibre [986].

705 Similarly to other insulating aggregates, researchers also focused on the effect of glass aggregates in
706 concrete blocks [459, 996-998] and structural concrete [999-1010]. According to the systematic review
707 study made by Mohajerani et al. [1011], concrete with foamed glass aggregates or expanded glass
708 aggregates has not been studied in detail. In addition, most of the studies are related to concrete
709 containing soda-lime glass or they did not mention the type of used glass. Moreover, the weakening
710 of the bond between cement paste and the glass aggregates [1003, 1006-1010], and expansion due
711 to alkali-silica reaction [1012, 1013], are two of the significant issues of this path. Nevertheless, ac-
712 cording to the data (experimental and literature) collected by Penacho et al. [1014], concrete and
713 mortars with satisfactory performance can be produced with glass sand. Nevertheless, they only did
714 short-term testing without performing the full alkali-silica reaction test.

715 Lightweight aggregates (LWA) can be manufactured (e.g. lightweight expanded clay, EC [1015, 1016]),
716 or sourced from nature (e.g. pumice [1017]), and waste products (e.g. (e.g. sludge ash [1018]., oil-

29
717 palm [852] and MIBA [1019] as lightweight aggregate). The manufactured-lightweight aggregates in-
718 crease the total EI of 1m3 of concrete [1020]. However, this path can still be considered sustainable
719 because it helps to build a safe structure with less weight [1021] and avoids thermal bridges in build-
720 ings [1022]. Further details on this path are given in §13.2. In addition, lightweight concrete may also
721 be produced with a lightweight steel system. However, studies on this path are very limited [1023-
722 1026], and mostly focused on sandwich systems.

723 5.6 Other types of aggregates

724 Concrete can also be produced with other non-conventional aggregates such as alkali-activated aggregates
725 (§4.6), magnetite/hematite/ferrock [1027-1030], pumice stones [1031, 1032], stone slurry [1033], ethylene-
726 vinyl acetate [1034, 1035], lead-zinc tailings [1036], mine tailings [1037], and biochar aggregates [1038].

727 6 Reduce the environmental impacts and resources use of water

728 The concrete industry can be considered one of the largest water-consuming sectors. As reported in
729 [1039], about 150 litres of water are needed per m3 of concrete. This value can be increased to 500
730 litres per m3 of concrete by considering washing out and losses during the production and transporta-
731 tion stages of concrete. The wastewater generated by this activity can be considered as a hazardous
732 substance due to the presence of heavy metals and its high pH [806]. Furthermore, mandatory chem-
733 ical boundaries, other limits and general guidance on the type and amount of impurities of concrete
734 mixing water are collected in [1040]. According to the literature, apart from potable water, the fol-
735 lowing main water types can be used in CBM.

736 6.1 Seawater

737 Seawater has been used in concrete in previous studies [1041-1043]. Romans made concrete that remains
738 intact for centuries by using lime, volcanic ash, aggregate and seawater [1044]. The mechanical strength
739 generally increases by incorporating seawater (as a raw material instead of potable water) in concrete,
740 especially at early ages (up to 7 days), and the opposite occurs at longer ages [1041-1043]. Besides some
741 attempts [1039, 1040, 1045-1047], it is urgent to contemplate the possibility of applying seawater in mixes,
742 especially in unreinforced concrete, where its consequences on reinforcement corrosion are not felt. Rel-
743 atively to freshwater, curing concrete with untreated seawater does not significantly affect its strength
744 [1043, 1048]. Thus, it is foreseen as a promising path to consume less freshwater.

30
745 6.2 Recycling water recovered from discarded ready-mix concrete

746 Similarly to seawater, water recovered from discarded ready-mix concrete has been used (i) for further
747 washing purposes [1049] and in concrete as a raw material [1050-1058] (mixing water) when it meets
748 the regulatory requirements for fresh concrete. A study [1059] collected the traditional and non-tradi-
749 tional methods of cleaning mixer trucks. In addition, by recycling water recovered from a ready-mix con-
750 crete plant [1057], concrete slurry waste can be also separated from water and used as recycled mate-
751 rials in concrete [1049, 1060, 1061]. Some treatment techniques seem to be promising [1062]. However,
752 studies on the durability performance of concrete with recycled water are very few.

753 6.3 Treated and untreated wastewater

754 The use of wastewater in concrete mixing is another strategy to decrease the impact of water [1063].
755 Wastewater such as sewage [1064-1066], industry [1067-1069] and greywater [1070, 1071] (grey-
756 water can be defined as any wastewater consumed by human activities in showers, bathtubs, laundry
757 machines, hand basins, and kitchen sinks, in schools, office buildings, households, etc. without any
758 inputs from toilets - [1072]) are the main types used in CBM. Several studies reported that the setting
759 time [1064], strength [1064, 1069-1071], entrained air [1064] and water absorption [1071] of CBM
760 may be unaffected by the use of treated wastewater. However, the use of untreated sewage water is
761 not recommended as mixing water in CBM composites [1064].

762 Apart from seawater, there are no studies on the effect of wastewater as curing water on the technical
763 properties of CBM. Besides a few case studies, there is no systematic review to show the effect of differ-
764 ent types of water (e.g. well water, tap water, mineral water, bore well water, seawater, agricultural
765 wastewater, rainwater and treated and untreated wastewater) on the technical properties of CBM.

766 7 Reduce the environmental impacts and resources use of reinforcement

767 Similarly to cement, aggregates and water, regular carbon steel rebars can be replaced with non-con-
768 ventional rebars such as bamboo [1073-1088], basalt rebars (§11.1.5), glass fibre reinforced-polymer
769 (FRP) rebars (§11.1.6) and carbon FRP rebars (§11.1.7). Other strategies such as stainless-steel rebars
770 (§11.1.1), low-carbon chromium reinforcing steel rebars (§11.1.2), epoxy-coated rebars (§11.1.3), and
771 galvanized rebars (§11.1.4) may not directly reduce the EI of concrete reinforcement. However, they
772 can be still considered as a sustainable solution due to the reasons mentioned in the first paragraph
773 of section 11, namely increasing the durability of reinforced concrete and consequently decreasing
774 yearly EI over the structure’s life cycle.
31
775 8 Material manufacturing

776 Most of the other strategies (§3-7) are related to the EI and energy consumption of concrete (e.g. mix
777 composition and technical properties of concrete) to lower its negative effects. Contrary to the men-
778 tioned sections, this chapter relates to the raw materials that have high EI and energy consumption.
779 In other words, the strategies that decrease the EI and energy consumption of manufacturing the main
780 raw materials used in concrete (e.g. cement - §8.1, aggregates - §8.2 and reinforcement - §8.4) are
781 discussed. Relative to the mentioned raw materials, the EI and energy consumption of water (e.g.
782 potable water) and admixtures (e.g. SP) are insignificant [155]. Thus, alternative pathways in the man-
783 ufacturing of these two materials are very scarce.

784 8.1 Cement production

785 As shown in Figure 10, production of cement can be classified in five stages, namely (i) raw materials
786 extraction, (ii) transport, (iii) fuel and energy consumption, (iv) calcination and (v) grinding. To achieve
787 lower EI and energy consumption in cement production, all the mentioned processes must be consid-
788 ered. As reported in [1089-1092], the CO2 emissions of cement production can be decreased through
789 each mentioned process:

790 (i) Extraction and crushing operations by considering best-practice mining (e.g. minimize essential equip-
791 ment use, conveyor belts and alternative fuels [1093-1096]), increasing machinery efficiency [1097], us-
792 ing recycled aggregates [540], reducing wear and using advanced lubricants in machinery [1098], and
793 considering renewable energy-powered mills [1099];

794 (ii) Transportation from one site to another by underground conveyor belts [1095] and with increased
795 efficiency [1100-1102]. This can be considered as a future plan because many quarries are usually no-
796 where near cement manufacturing plants;

797 (iii) Combustion by using alternative fuels [1103] such as oxy-fuel kiln [1090, 1104]) and belite cement (§4.5);

798 (iv) Decarbonation by using alternatives to decarbonation of limestone (reduce the total amount of
799 binder - §3, blended cement - §4.1-4.4, alkali-activated concrete - §4.6, Mg cement - §12);

800 (v) Comminution (e.g. milling, grinding, and chipping) using renewable energy [1105];

801 (vi) Substitute technology by prefabricating carbonate parts [1106, 1107] and green cement plant [1108].
802 In addition, some studies have developed an electrochemical process that can produce cement with
803 almost zero carbon-footprint [1109-1111].

32
804 Finally, it can be said that the assumption of concrete with near-zero-carbon cements can be made by
805 considering the strategy described in this section and CO2 sequestration by mineral carbonation.

806 8.2 Aggregates production

807 To decrease the EI and energy consumption of aggregates, the whole process of quarrying/mining
808 industry, shown in Figure 11, must be considered. In fact, each production process can be divided in
809 several sub-processes (e.g. resources extraction includes drilling and blasting, secondary breaking,
810 loading and hauling) and each of them needs to be studied to find a better solution in terms of sus-
811 tainability. However, apart from few attempts or some general recommendations made by these stud-
812 ies [1112-1124], there are very few studies on the optimization tools, source of the raw materials and
813 alternative production process, namely explosives, fuel, oils, electricity, equipment, vehicles, water,
814 rock type, management and transportation scenario. Thus, it is urgent to focus on this path.

7.0% 1.5% 50.0% 35.0% 5.0% 1.5%

Cement plant

(1500 °C)

Grinding
Extraction Transport Fuel & energy Calcination and/or Transport
treatment
Pyroprocessing
i ii iii iv v ii
815
816 Figure 10 - Activities affecting CO2 emission resulting from concrete production (adapted from [1089-1092])

817 As shown in Figure 11, for sustainability reasons, waste management can be made through recovering
818 or recycling CDW as aggregates. Despite the many gaps previously mentioned, most of the studies
819 have been focused only on this path, namely comparing the EI of natural and recycled aggregates [140,
820 155, 1125]. Bearing these results in mind, regardless of the transportation scenario, the difference

33
821 between the EI of natural aggregates and recycled aggregates may not be significant. In addition, some
822 studies showed that the EI of aggregates from mobile plants is less than that of fixed plants [1126].

Aggregate
(e.g. sand)

Natural Artificial

Shore and
Inland Recycled manufactured
offshore

Natural resources T. product T. CDW

Consumption
With and without T.

Resource Production T. industrial wastes Emissions

extraction
imports (e.g. Primary,
T. Raw materials secondary and
(e.g. Drilling and fine crushing, Recovery, recycling Waste
blasting, and sieving) (mobile or fixed plant) management
Secondary
breaking,
Loading and T. Mining waste, Waste
hauling) overburden etc. disposition

Transportation (T.); construction demolition waste (CDW)

823

824 Figure 11 - Different source of aggregates with their production stage (adapted from [1119, 1122])

825 8.3 Production of reinforcement

826 As schematically represented in Figure 12, the literature shows that iron and steel production (ironmaking,
827 steelmaking and steel products) are divided in 2-3 main steps, and each one can be made with different
828 procedures, machine and materials. Therefore, the number of routes to produce iron and steel is very high.
829 In other words, for each production step, companies have developed many pathways for iron and steel
830 production to decrease CO2 emissions and energy consumption of each process. As stated in various stud-
831 ies [1127-1129], the routes of iron and steel production can be identified in two main implementations:

832

34
 Ironmaking Steelmaking Steel products

Secondary raw
Preparation of raw Reduction device Intermediate Semi-finished
Initial raw materials materials and Steel oven type Application
materials type product products
reducing agent

Lump ore Coal Coke oven Blast furnace Direct reduced iron Basic oxygen furnace Coil Transport

Smelting reduction
Fine ore Oxygen Sintering Hot briquetted iron Electric arc furnace Plate Machinery
vessel

Recycled steel Coke Pelletising Rotary furnace Molten iron Pipe/tube Construction

Oil Shaft furnace Hot road Metal products

Fluidized bed
Electricity Reinforcing bar
furnace

Biomass Flash furnace Wire rod

Cyclone converter
Natural gas Profile
furnace

Hydrogen Electrolyser Cast steel

Methane

833

834 Figure 12 - Simplified iron and steel production routes (adapted from [1127-1130])

35
835 (i) “Best available technologies” that can highly decrease EI and energy consumption such as blast oxy-
836 gen furnace waste heat and gas recovery [1131-1134], coke dry quenching [1135-1140], continuous cast-
837 ing [1141-1150], optimized sinter pellet ratio [1151-1154], oxy-fuel burners [1155-1161], pulverized coal
838 injection [1162-1165], scrap preheating [1166-1168], sinter plant waste heat recovery [1131, 1169-
839 1171], stove waste gas heat recovery [1128, 1129] and top gas recovery turbine [1172-1174];

840 (ii) “Most innovative technologies”, whose use is not universal or at the moment are under development
841 and intended to be ready for commercialization such as carbon capture and storage - blast furnace/power
842 plant [1175-1179], COREX [1180-1184], direct sheet plant, FINEX [1185, 1186], HISARNA [1187-1189],
843 HYL/MIDREX/ULCORED [1190-1193] and top gas recycle blast furnace [1194, 1195]. Nevertheless, studies
844 show that there is still not a significant improvement in most proposed and available routes. Furthermore,
845 future research directions can be seen in [1127, 1194].

846 9 Concrete mixing

847 Concrete can be made in plants (ready-mixed) or on-site (mixer). Besides its high energy consumption,
848 concrete mixing affects the quality/homogeneity of concrete. Thus, both aspects must be considered in
849 terms of sustainability. Generally, many different mixers and mixing methods commercially available
850 have been used to produce concrete based on quality, cost, transportation scenario, volume of concrete
851 and rate of demand. As shown in [1196], different types of mixer and mixing methods must be consid-
852 ered to guarantee the quality of concrete (Figure 13). Some of the parameters shown in the figure have
853 been considered in the construction sector without any proper study and others have been studied by
854 researchers, e.g. operation design [1197], performance attributes [1198], mixing time and type of con-
855 crete mixer [1199], effectiveness of concrete mixers [1200, 1201], mixing energy [1202], workability and
856 mixing [1201], efficiency of mixer [1203], volumetric-measuring and continuous-mixing [1204], concrete
857 mixers and mix systems [1205, 1206], concrete mixes preparation [1207], sensor to monitor the effect
858 of the mixing procedure [1208], mixing degree [1209] and mix design using adaptive neural fuzzy infer-
859 ence systems [1210-1212]. Additionally, most of the studies are related to the quality of concrete. At-
860 tempts to decrease the energy consumption of each process are very scarce.

861

36
 Mixer

Mixer type Mixing method

Continuous
Batch mixers Mixing periods Mixer Efficiency
mixers

Horizontal or Performance attributes

Vertical (pan
inclined (drum (workability, air content
mixers)
mixers and density)
Loading period Mixing period Discharge period

Volume of mixture
Non-tilting Admixture Composition and
Centre shaft Water
drum accuracy to weigh them

Cement
Aggregates Mixing Energy (duration
Reversing drum Dual shaft
Other materials of mixing cycle)

Dry mixing Wet mixing

Counter-current Time Output Rate (rate of
Tilting drum
motion demand)

Planetary Wear and Tear,

motion Cleanness
862

863 Figure 13 - Mixer type and mixing method of concrete

37
864 10 On-site application

865 To build a concrete structure, most of the stages of construction, namely (i) pre-construction and pre-
866 placement meetings (ii) concrete ordering procedures (iii) transporting and receiving concrete (iv)
867 conveying, placing, consolidating and finishing concrete (v) concrete protection and curing require-
868 ments, must be considered to minimize potential problems, EI, energy consumption, cost and time to
869 build a structure. Nevertheless, since this path relates to the site itself and needs a bigger scale than
870 laboratory, individual studies with systematic data comparing the EI and energy consumption of tra-
871 ditional and non-traditional applications of the above mentioned stages are very rare. Among the
872 mentioned stages, digital concrete/3D printing has been recently focused by several research groups.

873 Automated and additive manufacturing (AM) techniques with traditional and non-traditional cementi-
874 tious materials, i.e. 3D concrete printing, shotcrete 3D printing and smart dynamic casting have been
875 rapidly adopted in many fields. The introduction and development of this technology in construction
876 happened in the early 21st century after Khoshnevis et al. [1213] proposed the contour crafting 3D print-
877 ing methodology for construction applications. They used robotic arms with a trowelled nozzle to create
878 a better finish of the printed concrete. This path can be considered one of the sustainability strategies
879 because it does not need manual labour and formwork. Though this path can be more economically
880 viable due to less manual labour, it is not so socially acceptable since it will mean fewer jobs. Further-
881 more, these two parameters’ cost may exceed 50% of the total cost of a concrete structure [1214]. Alt-
882 hough AM comprises many 3D printing techniques, only a few are feasible for construction purposes.
883 Two of the most promising examples are extrusion 3D printing technique [1215, 1216], and the binder
884 (inkjet) 3D printing technique [1217, 1218]. These are suitable and the most applicable techniques for
885 construction purposes [1219]. These techniques generally use mortar materials, and hence current lim-
886 itation are that they cannot use coarse aggregates in the mix design due to abrasion in the pump unit,
887 there are difficulties in feeding and the shape ability of concrete [1220-1224]. The other outstanding
888 research challenges in this field are compaction [1225-1227], the gaps between layers [1222, 1228-
889 1230], the printed material’s porosity [1231, 1232], and the nozzle of the printhead [1215, 1216, 1233,
890 1234]. In addition, studies on the durability performance of the printed CBM are very rare.

891 11 Increase the durability of reinforced concrete

892 One way to reduce EI of concrete is by increasing its durability. There are several direct (intrinsic

38
893 method) and indirect (extrinsic method) ways to achieve this strategy, namely by slowing down/stop-
894 ping rebars from corroding (§11.1), preventing penetration of aggressive agents to concrete (§11.2),
895 slowing down degradation of concrete (§11.3) and durability design (§11.4). Intrinsic methods involve
896 changing everything in the actual reinforced concrete either by changing concrete itself (e.g. additions,
897 mix design and cover) or using more resistant steel rebars. Extrinsic methods could probably involve
898 the use of paint or hydrophobic coatings among other methods. Generally, these strategies may in-
899 crease the initial cost and EI of the structure. However, it may also considerably reduce costs or EI
900 over the structure’s life cycle (long term) because the number of rehabilitations necessary in low-
901 performance concrete is higher than in high-performance concrete. Thus, the total cost of low-perfor-
902 mance concrete will be closer to that of high-performance concrete with every rehabilitation (Figure
903 14).

High-performance concrete
Low-performance concrete
Cost

Repair 1 Repair 2 Repair 3

Performance

Minimum performance level indicating the end of the service life

904 Time

905 Figure 14 - Cost and performance, including rehabilitation cost, versus service life for high- and low- performance concrete

39
906 11.1 Slow down/stop rebar corrosion

907 11.1.1 Stainless-steel rebars

908 The corrosion resistance and chloride threshold of stainless steel rebars (SSR) are about 800-1500 and 4-
909 24 times higher than those of the conventional bars, respectively [1235-1238]. Due to its importance in the
910 construction industry, several standards from EU [1239], UK [1240], USA [1241] and guideline reports
911 [1242-1244] have been developed. Generally, stainless steel can be divided in four types: (i) Austenitic
912 (most widely used type [1243] with high range of corrosion resistance [1242, 1245-1248]); (ii) Ferritic (rel-
913 atively to other SSR types, it has lower range of corrosion resistance [1242, 1249]); (iii) Austenitic-ferritic
914 (also called duplex stainless, is a combination between austenitic and ferritic SSR). Comparing to other SSR
915 types, austenitic-ferritic is cheaper and rated in the very high range of corrosion resistance [1242, 1245,
916 1250-1252]); (iv) Martensitic (it is not recommended to be used as reinforcement [1242] because it has
917 minimal ductility [1253]).

918 Generally, SSR are rarely used in the construction field because they may increase the initial cost of
919 the structure by as much as 6-10 times [1254]. However, it may also considerably reduce costs over
920 the structure’s life cycle (long term), especially for bridges [1255] and rehabilitation [1254, 1256]. In
921 addition, stainless-steel-clad rebar was introduced in the market in the past decade [1257]. They have
922 a conventional carbon steel core covered with a thin outer cladding of stainless-steel. They basically
923 perform similarly to solid stainless-steel rebars [1258]. However, they require following more de-
924 manding specifications for cutting and bending [1259].

925 Further studies are required to identify chloride threshold values of different types and grades of SSR,
926 and corrosion risk when it contacts carbon steel. In addition, researchers are only focused on Austen-
927 itic SSR [1246-1248]. It is clear that a review study needs to be made to understand recent develop-
928 ments in stainless steel.

929 11.1.2 Low-carbon chromium reinforcing steel rebars

930 High corrosion resistant reinforcing steel can be made either by solid stainless steel (high chromium
931 content, specified in AASHTO [1260] - §11.1.1) or by low-carbon chromium (low chromium content,
932 specified in ASTM [1261]). Even though this type of steel is identified in standard [1261], related studies
933 are very limited [1259, 1262-1268] and most of them are not associated with concrete reinforcement.

934 11.1.3 Epoxy-coated rebars

935 In this sub-strategy, conventional rebars are coated with epoxy to increase their corrosion resistance and
40
936 act as a physical barrier, and their chloride threshold value is above or equal to that needed to initiate
937 corrosion in regular steel rebars [1269-1271]. According to previous studies, epoxy-coated rebars (ECR)
938 with damage level of 0.004-0.50% may increase the corrosion resistance of rebars by 69-1762 times [1257,
939 1272, 1273], and their cost is lower than that of other rebars. However, their performance may not be
940 guaranteed because the coating may be damaged during bending, handling, placing, transportation, and
941 concrete casting. For example, recent studies [1272, 1274] show several cases where ECR-reinforced con-
942 crete (made in the past 30 years) failed due to corrosion issues. Therefore, an update of the service life of
943 structure containing ECR needs to be done, especially for structures made 30 years ago. So far, there is no
944 systematic review study on the performance of concrete with ECR. Even though there are some case stud-
945 ies on the application of ECR in bridge decks [1272], bridges [1275], marine bridges [1276], marine envi-
946 ronment [1277], marine substructures [1278], and tunnel structures [1279] relative to other sub-strategies
947 (§11.1.1, §11.1.4, §11.1.6-11.1.8), case studies on this path are very limited [1269, 1280-1284]. Further-
948 more, there are some attempts to increase the bond strength between ECR and concrete [1285, 1286],
949 and overcome the issue of damaging spots of the ECR by using self-healing epoxy coatings [1287].

950 11.1.4 Galvanized rebars

951 Another sustainable way to increase the reinforcement durability is by normal hot-dip galvanizing (zinc
952 coated/metallic coated) [1288-1300]. Even though the chloride resistance of galvanized rebars (GR) is
953 only 2-4 times higher than that of conventional rebars [1301-1303], it can be considered more cost-
954 efficient than ECR (§11.1.2) because it is more difficult to damage, even though it is 40% more expen-
955 sive than ECR [1289, 1291]. In low-performance concrete exposed to aggressive environments, galva-
956 nized rebar may not necessarily extend the service life of reinforced concrete [1304]. Similarly to ECR,
957 galvanizing decreases the bond strength between concrete and reinforcement [1305-1308]. Some re-
958 view studies have analysed the technical performance of GR in concrete and its application in the
959 construction industry [1304, 1309]. One way to promote using GR and offset its cost is by using it in
960 concrete (e.g. FA concrete) in which durability, namely carbonation, is an issue. However, studies on
961 the performance of GR in fully carbonated concrete are very limited [1310].

962 11.1.5 Basalt rebars

963 Basalt rebars are made with inert volcanic rock (basalt) and have been used as a fibre [1311-1321] for
964 strengthening purposes (secondary reinforcement) and as main reinforcement [1322-1326] in con-
965 crete. They have higher tensile strength than that of standard steel rebars [1322, 1325], but lower
966 modulus of elasticity that may significantly increase the deflection of a structure [1325]. Also, it has

41
967 higher resistance to corrosion and less weight relative to standard steel rebars [1321, 1327]. Addition-
968 ally, they are non-hygroscopic, and non-conductive thermally or electrically [1328, 1329]. Generally,
969 studies on basalt rebars as main reinforcement (mini bars) are very limited [1322-1326].

970 11.1.6 Glass fibre reinforced-polymer rebars

971 Similarly to basalt, glass FRP can be used in concrete as fibres [1330-1332] or main reinforcement
972 [1333-1336]. In this section, however, the focus is on their performance as the main reinforcement.

973 Some review articles were made to understand the performance of glass FRP on the following topics: in
974 aggressive environments [1337], structural applications [1337, 1338], strengthening [1338, 1339], near-
975 surface in reinforced concrete structures [1340], composites materials [1341, 1342], and the their chemical
976 and mechanical performance [1343]. Generally, the tensile strength of glass FRP rebars is higher than that
977 of standard steel rebars, but their modulus of elasticity is significantly lower. Thus, they may not be advis-
978 able for structural concrete, especially when it involves significant spans. Nevertheless, these rebars do not
979 corrode at all and, in terms of weight, glass FRP rebars are lighter than standard steel rebars. In addition,
980 they are thermally and electrically nonconductive.

981 The bearing capacity of structures with glass FRP rebars significantly decreases at elevated tempera-
982 tures [1333]. In addition, glass FRP is immune to both chloride contamination and many forms of
983 chemical-induced degradation [1344-1349]. Several studies concluded that columns with glass FRP
984 rebars have lower carrying capacity than those with standard steel rebars [1350-1352]. Furthermore,
985 bond between glass FRP rebars and normal [1353-1359]- and high- strength [1360-1364] concrete is
986 another issue of this type of reinforcement.

987 Generally, most of the studies focused on the performance of glass FRP rebars in columns [1365-1371]
988 and beams [1333, 1339, 1346, 1372, 1373]. However, studies on their performance in slabs are very
989 limited [1374]. In addition, most of the studies only focused on the present limitations of glass FRP
990 and not on future improvements.

991 The performance of concrete filled glass FRP circular tubes [1375-1380] or rectangular shaped FRP
992 cross-sections [1381-1384] is another application of FRP that researchers are now working on. How-
993 ever, knowledge on this path is still very limited.

994 11.1.7 Carbon fibre reinforced-polymer rebars

995 Carbon FRP is a type of composite material composed of polymer and carbon fibres. The carbon fibres
996 give the stiffness and strength, and the polymer works as a cohesive-matrix to protect and hold the

42
 997 fibres together. Even though carbon FRP rebars have been studied in many aspects such as durability
998 performance in general [1385, 1386], fire resistance [1387, 1388], stiffness [1389], flexural strength-
999 ening [1390-1392], tensile [1393], pull-out capacity [1394, 1395], bond strength [1396, 1397], shear
1000 behaviour [1398], and even GWP [1399, 1400], relative to glass FRP rebars studies on carbon FRP
1001 rebars are more limited [1385-1403]. Their seismic performance, and long-term behaviour and dura-
1002 bility when exposed to harsh environment have not been extensively studied yet.

1003 In addition, there are other types of FRP rebars such as aramid [1387, 1404-1408] and glass-carbon
1004 [1409] that can be used as reinforcement in concrete structure.

1005 11.1.8 Corrosion inhibiting admixtures

1006 The service life of concrete significantly depends on the corrosion rate of steel bars [1410, 1411]. Thus,
1007 several methods (§11.1.1-§11.1.7) have been proposed to prevent steel bars from corroding and to
1008 extend the service life of reinforced concrete structures as a result. Relatively to other techniques,
1009 corrosion inhibitors are one of the most efficient and appropriate methods due to their low cost, ex-
1010 cellent corrosion resistance effect, and easy application [1412-1418]. As defined in a ASTM standard
1011 [1419], corrosion inhibitors can be used to inhibit chloride-induced corrosion of reinforcing steel in
1012 concrete. Generally, there are no accurate data regarding the effect of corrosion inhibitors on the
1013 carbonation resistance of concrete, which is considered one of the two most influential factors on the
1014 service life of concrete and corrosion of rebars together with chloride penetration resistance.

1015 As shown in Figure 15, the corrosion resistance of concrete depends on the reinforcement concrete
1016 cover (time - to) and rebars corrosion resistance (time - t1). Each of these periods depends on different
1017 factors. Thus, corrosion inhibiting admixtures depending on their type (organic and inorganic) can af-
1018 fect either the concrete cover (reducing the permeability) or the rebars (forming a protective film) by
1019 (i) increasing the chloride threshold value (by improving the resistance of the passive-film or creating
1020 a barrier-film and extending its lifetime - t0 - as a result [1410]), (ii) decreasing chloride diffusion rate
1021 (increasing t0 [1410, 1411]), (iii) increasing the degree of chloride binding of concrete (decreasing the
1022 movement of ions on the metallic surface and increasing t1 [1410, 1411, 1420]), (iv) eliminating the
1023 dissolved oxygen in the pore system and preventing the ingress of oxygen (increasing t1 [1410]), or (v)
1024 increasing the electrical resistivity of the metallic surface (increasing t1 [1420]).

1025 Based on several studies [1421-1424], corrosion inhibitors can be classified based on mechanism (an-
1026 odic and cathodic, or both actions), type of chemical (organic and inorganic/mixed inhibitors) and ap-
1027 plication (either on the surface of hardened concrete or mixed during the production stage). Most
1028 examples of corrosion-inhibiting admixtures can be seen in the USA standard [1419, 1425].

43
1029

1030 Figure 15 - Corrosion process of structural concrete as a function of lifetime with and without corrosion inhibitors (adapted from [1410, 1411, 1420, 1426])

44
1031 Several studies [1410, 1411, 1420, 1426] simplified the electrochemical theory of corrosion, namely with
1032 and without the use of corrosion inhabiting admixtures. Under normal circumstances (non-protected
1033 metal surface), some parts of the rebars act as cathodes and others as anodes. With the presence of water
1034 and oxygen around the surface of rebar, corrosion will occur. Thus, the ultimate purpose of any corrosion
1035 inhibiting admixture or other protection systems (§11.1.1-11.1.4) is to stop fleeing/travelling electrons
1036 from the anodic area to cathodic area. This can be made by three protection mechanisms (i-iii):

1037 (i) Anodic inhibitors can be named passivation inhibitors or sacrificial inhibitors. In electrochemical terms,
1038 the anodic reaction of the anodic inhabiting admixture must be more active than the anodic reaction of
1039 the surface of steel bars. There are two types of anodic inhibitors, non-oxidizing ions (phosphate, molyb-
1040 dates, and tungstate) and oxidizing anions (nitrates, chromates, and nitrites), working in the presence and
1041 absence of O2, respectively. There are also inorganic-anodic inhibitors, such as chromates [1427], calcium
1042 nitrate [1428], nitrates [1422, 1429], sodium nitrite [1421], and trisodium phosphate [1430, 1431].

1043 (ii) Cathodic inhibitors may work similarly to anodic inhibitors by sacrificing themselves and producing
1044 a barrier film, and slowing the cathodic reaction on the surface of the metal (e.g. zinc, magnesium
1045 slats). Generally, anodic inhibitors are more effective than cathodic inhibitors because they generate
1046 less H2. As stated in [1420], in terms of chemical composition, corrosion inhibiting admixtures that
1047 mainly work as either anodic or cathodic mechanism can be identified as inorganic inhibitors. There
1048 are also inorganic-cathodic such as zinc oxide [1421, 1432].

1049 (iii) Mixed inhibitors (pore blocker - hydrophobic material that has polar groups charged positively and
1050 negatively) act on the cathodic and anodic areas. There are also organic - chemisorption and - physisorp-
1051 tion (mixed inhibitors) such as sodium ‘’nitrite+ zinc oxide’’ [1421], triethanolamine [1421], monoethan-
1052 olamin [1421], diethanolamine [1421], “disodium β-glycerol phosphate pentahydrate + sodium 3-ami-
1053 nobenzoate” [1433], “disodium β-glycerol phosphate pentahydrate + sodium N-phenylanthranilate”
1054 [1433], benzoate [1434], nitrite and ethanolamine [1435].

1055 There are some issues that need to be answered concerning this path. For example, (i) how do the corro-
1056 sion inhibitors work when concrete is fully carbonated or contaminated with salt-containing chloride ions?
1057 (ii) How long can the corrosion inhibitors protect the reinforcement of concrete structures? (iii) How to test
1058 corrosion inhibitors’ reliability in laboratory to achieve practice-related results? In addition, most of the
1059 previous studies used commercially available corrosion inhibitors without providing their composition.

45
1060 11.2 Slow down penetration of aggressive agents to concrete

1061 11.2.1 Shrinkage control

1062 Aggressive agents may penetrate concrete due to shrinkage cracks [1436, 1437]. To control the shrinkage
1063 of concrete, several strategies are proposed such as using shrinkage/crack-reducing admixtures (e.g. poly-
1064 oxyalkylene alkyl ether and propylene glycol [1425, 1438-1445]), controlling the mix design (w/b and aggre-
1065 gate/binder ratios [95, 1436]), and applying a surface treatment [1446]. In general, most of the materials
1066 used in concrete for self-healing can be included in this strategy, such as SCM (e.g. FA [742, 1447], SF [1448]
1067 and metakaolin [1448]), metallic/steel fibres [1449-1451], polypropylene fibres [1452, 1453], cellulose fibres
1068 [1454], polystyrene aggregate [1455], internal curing (e.g. light-weight aggregates (LWA) [1456-1458], su-
1069 per-absorbent polymers [95, 1458], water-saturated recycled porous ceramic aggregate [1459, 1460]), and
1070 expansive agents [1439, 1461-1464]. This strategy must be considered especially for self-compacting con-
1071 crete (SCC) due to the high risk of shrinkage caused by the low volume of coarse aggregates [1465].

1072 11.2.2 Self-healing concrete

1073 The self-healing (self-repairing) mechanism of concrete can be defined as the capability of concrete (or
1074 CBM) to repair its cracks by two processes, namely (a) autogenous and (b) autonomous (Figure 16). Several
1075 review studies can be seen on this path [1466-1475], but there are many contradictory statements in terms
1076 of the classification of the two mentioned process. This may have happened because some materials can
1077 be used for both purposes (autogenous - as a main healing material and as a secondary healing material to
1078 protect the main healing material).

1079 (a) In autogenous self-healing (a natural phenomenon, spontaneous and self-created, that occurs
1080 without the presence of external/artificial phenomena), cracks may heal after some time due to (i)
1081 expansion of hydrated cementitious matrix, (ii) carbonation of calcium hydroxide, (iii) impurities pre-
1082 sent in water, and (iv) ongoing hydration of unreacted cement [1476]. This healing mechanism occurs
1083 in the presence of the materials that are not specifically designed for self-healing [1477]. In fact, they
1084 are added to concrete for other purposes, i.e. durability or strengthening.

1085 (b) Contrary to autogenous self-healing, autonomous self-healing can include any technique that uses
1086 cementitious materials only for healing cracks. Bacteria-based (with and without shell) and capsule-
1087 based (polymer-based containing liquid healing agents) are the most common techniques in this path,
1088 but have not been applied in practice. Apart from the mentioned techniques, fungi, shape memory ma-
1089 terials, and external supply of healing agent can be also classified as autogenous self-healing (Figure 16).

46
 Self-healing (repairing) cement-based material

Autonomous self-healing Autogenous self-healing

Without shell

Bacteria - without shell With shell Cement

Fungi Self-healing coating Supplementary cementitious materials
Encapsulation of chemical agents Vascular system Super absorbent polymers
Shape memory materials Electrodeposition method Nanomaterials Crystalline chemical admixtures
External supply of healing agent Curing of material in bacterial culture Mineral admixtures Expansive admixtures
Spraying/injection of bacteria
Fine particles:
Metabolic Enzymatic Swelling Continued Calcium Broken of Originally
conversion ureolysis hydration carbonate from fracture in the
Of organic acid formation surface water
Most common mechanism

Bacteria-based Capsule-based Physicochemical Mechanical Mixed

1090

1091 Figure 16 - Self-healing strategies in cement-based materials (adapted from [1466-1474])

47
1092 11.2.2.1 Autonomous self-healing

1093 11.2.2.1.1 Bacteria as self-healing agent

1094 Bacteria are incorporated with cementitious materials as a potential self-healing agent because they
1095 motivate the precipitation of CaCO3 as a crack-healing agent. Based on the metabolic processes, four
1096 types of bacteria can induce CaCO3 precipitation, namely (i) aerobic respiration [1478-1487], (ii) nitro-
1097 gen cycle [1478-1480, 1488-1495], (iii) photosynthesis [1496-1498], and sulphur cycle [1496, 1497,
1098 1499]. Further details on each of these bacteria types are shown in [1474].

1099 In terms of application, bacteria can be directly added to the cementitious materials without shells [1500-
1100 1511] or they can be added with shells (encapsulation material) such as calcium alginate [1512], ceramsite
1101 [1513], diatomaceous earth [1514], geopolymer [1515], hydrogel [1516], iron oxide nanoparticle [1485,
1102 1517, 1518], expanded clay (EC) [1486, 1519], melamine-based [1520], polyurethane [1487], silica gel
1103 [1487], and zeolite [1521]. Compared to the direct addition of bacteria, the long-term viability of the bac-
1104 teria with the encapsulation technique is higher because it protects bacteria from the high pH of the ce-
1105 mentitious materials [1470]. Moreover, bacteria can be externally added to concrete (§11.2.2.1.4).

1106 11.2.2.1.2 Fungi

1107 Fungi can be multicellular or single-celled organisms such as yeasts and moulds. Some studies show
1108 that fungi can also fill the cracks in cementitious materials. However, studies on this path are very
1109 limited [1468, 1522, 1523]. Thus, as reported in [1524], the mechanism of fungi to fill cracks has not
1110 been fully understood yet.

1111 11.2.2.1.3 Encapsulation of chemical agents

1112 Encapsulation can be made by filling the capsule materials with a healing agent, i.e. bacteria
1113 (§11.2.2.1.1) or chemical agents [1466, 1525-1527]. In this section, the focus is only on the method
1114 with chemical agents. The self-healing-based encapsulation can be made with either micro- [1466,
1115 1472, 1477] or tubular- [1466, 1528, 1529] capsules (the tube can be similar to a vascular system but
1116 it is filled with the healing agent and both ends are closed) filled with a chemical agent such as cy-
1117 anoacrylate [1528, 1530], epoxy [1530-1533], acrylic resin [1532], sodium silicate solution [1534],
1118 “methyl methacrylate with triethylborane as catalyst’’ [1535], tung oil [1536], calcium hydroxide
1119 [1536], and polyurethane [1537]. Additionally, the capsule material can be made with glass [1528,
1120 1530, 1533, 1537, 1538], Perspex [1533], urea formaldehyde formalin [1532], gelatine [1532, 1536],
1121 formaldehyde [1531], polyurethane [1534], silica gel [1535], ceramics [1536, 1537], and others [1474].

48
1122 11.2.2.1.4 External supply of healing agent

1123 The external supply of healing agent can be related to many paths. Nevertheless, the paths mentioned in
1124 this section are related to the techniques that spontaneously work when cracks occur. This strategy can be
1125 made with hollow fibres and is called a vascular system. In this system, the healing agent is supplied to
1126 concrete by an external source through the hollow tubes previously installed in concrete at the fresh stage
1127 [1528, 1538-1541]. Generally, the tube can be made of glass [1466, 1542] or carbon fibre-reinforced plastic
1128 [1466]. This system can be made with single-channel when only one healing agent is used and multiple-
1129 channel when the healing agent involves the reaction of two components [1470]. This strategy is feasible
1130 only at laboratory scale and it may not be cost-efficient for bigger scales because it requires a long piping
1131 system to cover the entire structure [1470] and it is difficult to release the agent from the pipe [1466].
1132 Therefore, capsule-based self-healing can be considered as an alternative method.

1133 Apart from the vascular system, this strategy can be also made by curing of material in bacterial cul-
1134 ture [1543], spraying of bacteria [1544], injection of bacteria [1545, 1546], electrodeposition method
1135 [1547-1553], and self-healing coating (§11.2.3).

1136 11.2.2.1.5 Shape memory materials as self-healer

1137 Shape memory materials (SMM), i.e. alloy wire [1473, 1474, 1554-1556] or polymers [1473, 1474,
1138 1557, 1558] as reinforcing bar, are effective to reduce the size of cracks and increase the resistance of
1139 concrete to any damage actions due to their super-elastic behaviour [1559-1567]. However, the cracks
1140 cannot be filled and still exist. SMM can be activated by electricity or heating to generate effective
1141 stress to facilitate energy dissipation and control cracks [1568-1570]. SMM fibres can be straight or
1142 dog-bone shaped, with and without paper wrapping in the middle [1561]. A systematic review study
1143 must be done to show the types of materials that can be used for this purpose.

1144 11.2.2.2 Autogenous self-healing

1145 11.2.2.2.1 Supplementary cementitious materials

1146 Apart from cement, many of the SCMs may work as autogenous self-healing materials [1472]. For that
1147 purpose, researchers have studied the feasibility of slag [1571-1584], FA [332, 1571, 1573, 1575, 1578,
1148 1580, 1584-1601], lime [1596, 1602, 1603], silica [1576, 1582, 1604], and metakaolin [1582] for moni-
1149 toring autogenous crack healing in cementitious materials.

1150 11.2.2.2.2 Super absorbent polymer

1151 Super absorbent polymer (SAP) can absorb a great quantity of liquid and swell significantly to form an

49
1152 insoluble and soft gel [1466, 1477]. It may work as a direct physical blocking effect after exposure to water
1153 and swelled, or it may work as an internal curing system and motivate autogenous healing [1466, 1605].
1154 Although this strategy causes autogenous healing, it can be also considered as autogenous because these
1155 materials are also added to concrete and do not belong to a typical mix design. For that purpose, it has
1156 been used in CBM [1606-1616]. Nevertheless, uncoated SAP may absorb a part of concrete mixing water
1157 during the fresh state and generate a considerable amount of porosity in hardened concrete. To overcome
1158 this issue, the SAP particles are encapsulated with a shell to resist the mechanical stresses of mixing proce-
1159 dure and become fragile enough to be broken when a propagating crack passes through them [1605].

1160 11.2.2.2.3 Expansive and crystalline admixtures

1161 Another way to achieve autogenous self-healing can be through (i) expansive admixtures such as calcium
1162 sulpho aluminate [1617], MgO [1594, 1618], CaO [1618-1620], anhydrite[1617], bentonite [1618, 1621];
1163 generally, they react with calcium hydroxide to procedure expansive products (e.g. calcium hydroxide,
1164 ettringite, magnesium carbonate and magnesium hydrate) and consequently fill the cracks; (ii) crystalline
1165 chemical admixtures that consist of hydrophilic active chemicals particles [1425] such as crystalline catalysts
1166 [1617, 1619, 1622, 1623], sodium silicate [1624-1626], colloidal/active silica, sodium carbonate [1617,
1167 1627], sodium monofluorophosphate [1627]. According to a previous study [1474], crystalline admixtures
1168 such as ethyl silicates sodium bicarbonate and lithium carbonate can be used for the same goal. In terms of
1169 application, the mineral admixture can be added to concrete by encapsulation [1618, 1624-1626] or direct
1170 [1623] use or only by dipping the sample in a solution [1628]. Studies on this path, namely using crystalline
1171 chemical admixtures in concrete, are very limited and, as presented by [1474], there might be other mate-
1172 rials (e.g. ethyl silicates sodium bicarbonate and lithium carbonate) to be used for the same purpose.

1173 11.2.2.2.4 Nanomaterials-based self-healing concrete

1174 As any other autogenous self-healing strategies, the main purpose of using nanomaterials is to act as a
1175 crack bridging agent and in concrete as filler and enhance concrete’s performance [524, 1629]. According
1176 to a review study [1473] on nanomaterials-based self-healing concrete, nanomaterials in self-healing con-
1177 crete are added to control the corrosion of steel bar. Generally, several types of nanomaterials have been
1178 used in concrete such as carbon nanotube (CNT) [1630-1643], polycarboxylates [1644], titanium oxide
1179 [1645], nanokaolin [534], nanoclay [534], nanoiron [1646], nanosilver [1646], and graphene [1647, 1648].

1180 11.2.2.2.5 Other techniques

1181 The expression “smart concrete” can include most of the autogenous and autogenous self-healing
1182 strategies. Several studies on so-called smart concrete use carbon fibre [1649-1654], shape memory

50
1183 alloy [1565, 1655], phase change materials [1656] and sensors fabricated using nanotubes or others
1184 hybrid fillers [1657-1659].

1185 11.2.3 Surface protection

1186 According to review studies [1660, 1661], in terms of chemical composition, surface protection agents
1187 can be classified as: (i) organic, which is the most commonly used and effective technique to protect
1188 concrete [1662]; however, its service life is short, and it may not easy to remove [1660-1662]; (ii)
1189 inorganic, such as sodium silicate solution (most common), lithium silicate, fluosilicates and potassium
1190 silicates, which have been also used to protect the surface of concrete [1660, 1661, 1663, 1664].

1191 In terms of mechanism, based on the strategies given in various studies [1665] [1660, 1666-1670] and
1192 a standard [1671], surface protection can be divided in four main groups (i) surface coating, (ii) multi-
1193 functional surface treatment, (iii) pore blocking surface treatment, and (iv) hydrophobic impregnation.

1194 11.2.3.1 Surface coating

1195 Surface coating creates a continuous polymer film that works as a physical barrier to stop aggressive
1196 agents penetrating into CBM [1660, 1672, 1673]. As reported by [1660], in terms of composition, sur-
1197 face coating can be divided in three groups: (i) traditional polymer coatings such as epoxy resins [1674-
1198 1684], acrylic [1685-1688] and polyurethane/asphaltic [1689-1696]; (ii) polymer nanocomposite coat-
1199 ings such as polymer-clay [1697-1700], silane-clay [1701], polymer-silica [1702-1704]; as confirmed in
1200 [1660], polymer-Al2O3 as coating has potential for this path but it has not been investigated yet; (iii)
1201 mixed coatings, such as polymer modified cementitious coating [1673], acrylic rubber surface coating
1202 [1705], and alkali-activated materials coating [1706-1710].

1203 11.2.3.2 Hydrophobic impregnation

1204 By coating the surface of hardened concrete with hydrophobic agents (water repellent) such as silane
1205 and/or siloxane [1660, 1701, 1711-1713], the surface of interior-pores of concrete can be increased
1206 increasing the surface contact angle between concrete and liquid to more than 90° [1714]. Thus, this
1207 technique inhibits water and other aggressive liquid from penetrating through the pores of concrete
1208 by capillarity, even though humidity can enter or exit. This strategy can be also applied by incorporat-
1209 ing nanoparticles [1715, 1716], acrylic-silicon resin [1717], micro silica particles [1718], GGBS [1719],
1210 and stearic acid emulsion [1720].

1211 Recently, superhydrophobic coatings have also been developed by researchers. They can include ammo-
1212 nium polyphosphate[1721], calcium carbonate nanoparticle [1722], candle soot [1723-1726], carbon

51
1213 black/polybutadiene elastomeric composite [1727], cyanoacrylates [1728], epoxy resin [1729], graphene
1214 oxide/diatomaceous earth/polydimethylsiloxane [1730], polyelectrolyte complexes [1731], silver nanopar-
1215 ticles [1732], SiO2 [1733, 1734], TiO2 [1735, 1736], wax [1737], and RHA [1738-1740].

1216 11.2.3.3 Pore blocking surface treatment

1217 This strategy intends to block the capillary-pores in the concrete surface to increases its watertight-
1218 ness and hardness. For that purpose, fluosilicate [1741-1743] and silicate-based solutions (e.g. sodium
1219 silicate [1669, 1742, 1743], calcium silicate [1744]) have been used as an effective agent to block ca-
1220 pillary-pores in concrete surfaces.

1221 Electro-kinetic nanoparticle treatment [1745, 1746] and brushing nano-SiO2 [1747, 1748] and nano MgO
1222 [1660, 1749] can be also used as a pore blocking surface treatment. Additionally, this strategy can be
1223 also be made with self-healing coating by using epoxy coating containing microencapsulates [1750-
1224 1752], fibres distributed in a shape-memory epoxy matrix [1753], hydrogel coatings [1754], polymer
1225 coatings [1755-1758]. Although the results of this path are very promising, there are only few studies
1226 focused on this strategy.

1227 11.2.3.4 Super skin concrete

1228 The term super skin concrete can be defined as a thin ultra-high-performance concrete used to protect
1229 and be filled with ordinary concrete. It may resist the ultimate load of the structure and improve du-
1230 rability. It can work as a typical concrete-filled steel [1759-1761] or FRP [1762] tubular cross-section.
1231 This strategy is normally used in rehabilitation to cover old concrete. However, there are only few
1232 scientific works on this path for beams [1763] and columns [1764].

1233 11.3 Reduce degradation rate of concrete

1234 11.3.1 Alkali-aggregate reaction

1235 Generally, aggregates can be considered an inert material from a chemical point of view. However,
1236 some of them may react with the alkali-hydroxides in concrete, resulting in expansion and cracking
1237 over time. The alkali-aggregate reaction may induce concrete damage in two forms: alkali-silica reac-
1238 tion (ASR) and alkali-carbonate reaction (ACR).

1239 ASR damages concrete due to the presence of reactive silica in the aggregate, alkalis mainly from ce-
1240 ment, and moisture [1765-1768]. To prevent or mitigate ASR, the following paths have been consid-
1241 ered: (i) SCMs, namely FA, are the most common solution to prevent ASR [1769-1773]. Other SCMs,
1242 such as SF [1769], GGBS [1773-1775], metakaolin [1776] and other calcined clays, RHA [1777] and

52
1243 natural zeolites [1778], can be also used for the same purpose; (ii) chemical admixture, such as lithium
1244 salt [1779, 1780], air-entraining admixtures [1779, 1781], hydration controller [1782, 1783], ilanes,
1245 siloxanes, and silicofluorides [1784, 1785], and phosphate [1786]; (iii) using nonreactive aggregates
1246 complying with standards ASTM C294 [1787] and C1293 [1788], CSA A23 [1789]; BS 7943 [1790],
1247 RILEM AAR [1791], AASHTO PP65 [1792] and other standards collected in a review study [1766]; (iv)
1248 limiting the total alkali content of concrete to 1.8-3 kg Na2Oe per m3 [1765, 1788, 1789]. Apart from
1249 cement, alkalis may have also come from some specific SCM, aggregate, chemical admixtures, recycled
1250 water and outer sources such as de-icing salts and seawater [1765, 1766, 1793].

1251 Relatively to ASR, ACR damage in concrete is rare and it mainly happens when a specific type of ag-
1252 gregates (dolomitic rocks) or clay is present in the matrix [1794, 1795]. In terms of mechanism, there
1253 is no consensus on how ACR affects concrete [1796]. Future paths to prevent ASR and ACR damage in
1254 concrete have been identified in [1766].

1255 11.3.2 Freeze-thaw resistance

1256 Water expands when it freezes. Accordingly, as water inside concrete pores freezes, its volume increases
1257 and consequently generate pressure. This may rupture and dilate the concrete voids if it is higher the ten-
1258 sile strength of concrete. As reported in [1797], frost resistance can be improved in four ways: (i) hindering
1259 crack propagation by using CNT [1798, 1799], PVA fibre-reinforcement [1800, 1801], graphene oxide [1802,
1260 1803] nano silica [661] and nano TiO2 [1804]; additionally, there are some novel surfactants that can work
1261 as air entraining agents [1805, 1806]; (ii) refining pores and decreasing the porosity of concrete by using
1262 SCMs (e.g. FA [1807], SF [1808, 1809], metakaolin [1810, 1811], RHA [1812, 1813], GGBS [1811, 1814]) and
1263 fillers; (iii) reducing water absorption by using hydrophobic admixtures in concrete [1797]; (iv) introducing
1264 additional space for ice-expansion in concrete by adding air-entraining admixtures [1815, 1816].

1265 11.3.3 Resistance to other physical and chemical attacks

1266 The effect of aggressive soils (sulphates and other salts), abrasion, marine salt exposure, soft water and
1267 cyclic wetting-drying must also be considered in advance to predict the service life of concrete. For exam-
1268 ple, a study [1817] collected all current specifications and codes and showed requirements for each of the
1269 mentioned issues in various standards in America, Europe, Australia, Canada, and China. To improve dura-
1270 bility regarding the mentioned issues, industrial SCM (§4.2), slowing down or stopping penetration of ag-
1271 gressive agents (§11.2) and unconventional reinforcement (§11.1) have been used in concrete. Addition-
1272 ally, the durability design (§11.4) is the most important factor to overcome the mentioned issue.

53
1273 11.4 Durability design

1274 The factors that affect durability design are shown in Figure 17. All the factors at the material level,
1275 structural level, external factors and design stage must be considered in advance to obtain a durable
1276 design. In other words, such design may not increase the service life of a new concrete structure, but
1277 rather it guarantees/controls a given service life of concrete by providing a baseline for the engineer-
1278 ing judgment of the most relevant factors affecting durability of concrete. Nevertheless, durability
1279 design has been considered as key to improve concrete’s sustainability [1818] and it should be con-
1280 sidered based on concrete’s application.

1281 Besides quality control and quality assurance, reliability of the considered data (input parameters)
1282 [1819] [1820] and of modified models (e.g. DuraCrete [1821], Life-365® [1822], STADIUM®[1823], fib
1283 Bulletin 34 [1824], concrete Works [1825] LIFEPRED [1826], ClinConc [1827], DuraCon [1828], durabil-
1284 ity Index [1829] and approach [1830]) is required to estimate the service life of concrete [1831, 1832].
1285 Future paths for durability design of concrete structures have been identified in [1817, 1832, 1833].

1286 12 CO₂ mineralization and utilization (carbon capture and storage)

1287 The greenhouse gases emission generated by the cement industry can be decreased by capture (storage
1288 and sequestration) of CO2 directly from cement plants (§8.1) or by CO2 sequestration by mineral carbon-
1289 ation. Generally, alkaline earth (e.g. Mg and Ca), alkali (e.g. K and Na) and other metals such as Zn, Cu,
1290 Ni, Co, Fe and Mn can be carbonated to capture CO2. Nevertheless, most of these elements are either
1291 very expensive or rare and not suitable to be used as feedstock for CO2 mineralization. For example,
1292 alkali metals have a great affinity to CO2 and they are very soluble for CO2 sequestration, especially in
1293 the long-term. In addition, although there is a substantial amount of Fe in nature, it is not suitable to be
1294 carbonated because it involves valuable iron ore. In fact, Mg (e.g. serpentinite [1834-1836], dunite- oli-
1295 vine [1837, 1838] and basalt [1839] rocks) and Ca (wollastonite [1840-1842] and basalt [1839] rocks) are
1296 the most suitable elements to capture high amounts of CO2 because they are more common in nature
1297 than other potential metals [1843]. As reported in [1844, 1845], CO2 capture in CBM can be made by
1298 carbonation of calcium hydroxide [1844, 1846], calcium silicate hydrates [1847-1851], calcium sulfoalu-
1299 minate hydrates [1852, 1853], cement clinker minerals [1854-1856], and magnesium-derived hydrates
1300 [1857, 1858]. CO2 sequestration is affected by exposure conditions (e.g. CO2 partial pressure/content
1301 [1849, 1859], temperature [1860, 1861], CO2 source [1862, 1863]) and properties of cement-based ma-
1302 terials (e.g. water content [1864-1866], chemical composition [1844, 1867], particle size and surface area
1303 [1845, 1866], porosity and permeability [1868, 1869]).

54
1304
1305 Figure 17 - Durability design, quality assurance and operation of new concrete in severe environments (adapted from [1797, 1817, 1833, 1870-1873])

55
1306 Concrete can be cured in a carbonation chamber [1874, 1875] or using other novel techniques such as
1307 aqueous CO2 solution [1876] to promote and accelerate CO2 sequestration. Besides magnesium [1107,
1308 1857, 1877-1880] or calcium -rich materials [1881], SCMs [130, 1845, 1858, 1877-1880, 1882-1884] (mostly
1309 FA), cement waste [1885], CDW [1886], and nano-materials [1887] can also be used for CO2 sequestration.

1310 Critical issues and areas for further investigation in this path have been identified in several studies
1311 [1089, 1839, 1843, 1845, 1888-1892]. To link this path with industry, recycled aggregates made with
1312 concrete containing materials rich in Mg or Ca can be used as a filter to sequestrate CO2 and other
1313 greenhouse gases generated by the industry. For that purpose, a chamber with a given pressure and
1314 humidly needs to be built and filled with the aggregates. Then, the greenhouse gases can be passed
1315 through this chamber in order to be sequestrated by the aggregates before they are released.

1316 13 Thermal conductivity improvement and energy saving

1317 The energy expenditure in a building throughout its service life can be far greater than that expended
1318 for its construction. Saving energy in the form of heat or air conditioning for many years is one of the
1319 best approaches to achieve sustainability. One way to decrease the amount of heat transfer through
1320 conduction and of energy consumption of buildings is by reducing the thermal conductivity (k-value)
1321 of concrete. As reported in [1893], the thermal conductivity of concrete may be affected by the fol-
1322 lowing parameters (§13.1-13.4).

1323 13.1 Moisture content and temperature’s impact

1324 Since the k-value of air is 25 times lower than that of water [1894, 1895], the k-value of concrete with
1325 high moisture content or in the SSD state is higher than in the oven dry state [1896-1899]. For exam-
1326 ple, a study [1900] showed that the k-value of SSD concrete is 50% higher than that of dry concrete,
1327 and other studies showed that the k-value of concrete increases by 6% [1901] and 5% [1902] with 1%
1328 increment in unit weight and moisture content, respectively. In addition, the k-value of concrete sig-
1329 nificantly falls as temperature increases [1899, 1903-1907].

1330 13.2 Type and proportion of aggregates and other additional materials

1331 Since aggregates have the lion share of the volume of concrete, the k-value of concrete significantly
1332 changes by using different types and proportions of aggregates. For example:

1333 (i) Natural aggregates such as basalt [1908], limestone [1908], siltstone [1908], or others contain large
1334 amount of the following minerals: quartz [1908, 1909], feldspar [1909], (metamorphic) gneiss [1909],

56
1335 amphibole/pyroxene [1909] and iron ore magnetite [1909];

1336 (ii) Lightweight materials (rounded or angular/irregular), mainly EC (commercial names Leca [1022],
1337 Argex [1022, 1910]), expanded slate (commercial name Stalite [1022, 1910]), expanded shale (com-
1338 mercial name Asanolite [1910]), pumice [1911-1913] and sintered FA (commercial names Lytag
1339 [1022]). There are few studies on the following LWA, namely perlite [1914, 1915], cenospheres [1916,
1340 1917], polyurethane foam [1918, 1919], diatomite [1911], expanded glass [1920, 1921], silica aerogel
1341 (SA) [1922-1925], high-impact polystyrene [1926], iron ore tailings [1916], wood shavings [1927], man-
1342 ufactured plastic aggregate [1928], dry lime-hemp [1929-1932], and biochar [1038];

1343 (iii) AWAF such as oil palm shell [1933], palm fibre [1934], coconut shell [858], corncob [1935] rice husk
1344 [867, 1936-1938], tobacco wastes [870], sheep wool fibres [1939]. Studies on this path are very scarce;

1345 (iv) Phase change material and others.

1346 Phase change materials (PCM) are normally placed inside a building to reduce its energy consumption and
1347 enhance indoor thermal comfort due to their potential to store and absorb heat [1940, 1941] in the phase
1348 change from liquid to solid and vice versa, during exothermic and endothermic phenomena [1942]. Based
1349 on the review study [1943], PCM can be classified as organic (paraffin and non- paraffin) and inorganic
1350 (hydrated salts). Recently, some studies [1943-1945] [1656, 1946-1949] showed that PCM can be used in
1351 CBM to decrease their k-value. Nevertheless, further studies need to be made to see whether there are
1352 any negative effects of the PCM on other technical properties of CBM. Other cementitious materials that
1353 increase the reflection of sunlight and absorb less heat [1950, 1951], and soil-based materials [1952-1954]
1354 can be other promising paths within this strategy.

1355 13.3 Binder content and type

1356 Binder content and type may also affect the k-value of CBM. Nevertheless, their influence is not sig-
1357 nificant compared to other factors mentioned in other sections. Generally, the most often used SCMs
1358 within this path are FA [1910, 1955, 1956], SF [1956-1958] and slags [1955, 1958]). In addition, SCMs
1359 (e.g. CBA) can be also used as aggregates [1959]. A study [1956] showed that the k-value increases
1360 with increasing binder content of concrete.

1361 13.4 Natural fibres

1362 Natural fibres (NF) can also be used in CBM, most commonly to improve their thermal insulation [1934].
1363 However, most of the previous studies [1960-1967] concluded that the technical properties of the ce-
1364 mentitious materials decrease as the incorporation ratio of NF increases. According to these studies

57
1365 [1968-1971], NF can be divided in two main groups: (i) plant/lignocellulosic fibre such as seed (e.g. cotton
1366 [1972, 1973] and kapok [1969]), stalk (e.g. tree wood [1974-1976], wheat [1977], rice [867, 1978] and
1367 barley [1979] straws, and crops such as bamboo [1980] and corn [1981]), leaf (e.g. abaca [1982], agave,
1368 banana and sisal [1983-1986]), fruit (e.g. coir/coconut [1987]), blast/stem-skin (e.g. jute [1988], flax
1369 [1989, 1990] and hemp [1929-1931, 1991, 1992] and banana [1991]), grass (e.g. bagasse [1993], ele-
1370 phant [1977] and bamboo [1994]), root (e.g. broom root [1995, 1996]), and other by-products of plant
1371 (e.g. cellulosic [1997], and cellulose pulp [1998]); (ii) animal fibre [1999] such as animal hair (wool
1372 [1939]), silk and avian (feathers of birds [2000]); further development within this path are summarised
1373 in [1969]; (iii) mineral fibres (ceramic [2001, 2002], asbestos [2003, 2004], and metal [2005-2008]).

1374 In addition, NF can be also used in composites materials. For example, a natural fibre reinforced polymer
1375 composite has been developed using sisal [2009-2013], hemp [2014, 2015], short jute [2016] and flax
1376 [2017, 2018]. A study [2019] collected examples of the application of natural fibre reinforced polymer
1377 composites in the industry and reported that it can be used instead of asbestos [2020, 2021], and is
1378 ideal to be used in roofs, ceilings and walls due to its lightweight.

1379 13.5 Density and microstructure

1380 Apart from the parameters shown in §13.2-13.3, the k-value of CBM is significantly affected by w/b
1381 [1955], volume of aggregates [1955], size and proportion of sand and gravel [1900, 1955] (e.g. no-
1382 fines concrete [2022-2024]), porosity [1908, 1955] (e.g. foam concrete/aerated concrete [2025-
1383 2031]), and nature of the pores [1908]. All these parameters directly affect the density of CBM. As
1384 shown in Figure 18, regardless of the type of used materials (i-iii), it can be said that density of concrete
1385 is the major parameter to change the k-value of any type of CBM (paste, mortar and concrete).

1386 Figure 18 shows that ACI committee 213 R-03 model (k-value = 0.0864e0.00125·density)) can be used as a
1387 reliable model for any type of materials. By comparing the actual and calculated k-value (Figure 18-
1388 inset graphs), the coefficient of determination (R2) with the ACI committee 213 R-03 model (upper
1389 inset graph) was 0.66. This coefficient can be increased to 0.77 (lower inset graph) by modifying the
𝑤/𝑏
1390 mentioned model (0.85·(0.0764- 40 ) e(0.00141*density*(60%+w/b)), namely by considering the w/b ratio.

1391 In general, most of the studies are focused on the effect of various parameters (e.g. aggregates, SCM
1392 and w/b) on either SSD or oven-dried concrete. However, in a real situation, these two states rarely
1393 occur in CBM. Therefore, as reported in [1893], the focus of the future studies within this path must
1394 be on the effect of humidity in concrete for any selected parameters.

58
 Thermal conductivity Alkali-activated concrete based CFA and Oil palm shell foamed
Concrete containing CFA Concrete containing SF
Concrete containing SF and f GGBS Concrete containing SF andf CFA
Concrete containing GGBS Concrete containing CFA and GGBS
Concrete containing CNT Concrete containing LWA/Argex
Concrete containing LWA/EC Concrete containing LWA/expanded shale
Concrete containing LWA/Leca Concrete containing LWA/Lytag
Concrete containing LWA/pumice Concrete containing LWA/Stalite
Concrete containing RHA Concrete containing silane and SF
Concrete containing wooden aggregate Concrete with brass shavings
Concrete with copper wires Concrete with micro PCM
Concrete with PCM dispersion Concrete with PCM pellets
Foamed concrete Graphite and magnetite concrete
Graphite concrete Mortar containing CFA
Mortar containing SF Mortar containing GGBS
Mortar containing EC Mortar containing ECG
Mortar containing high -dense SA and EC Mortar containing high -dense SA, ECG, EC, L and CFA
Mortar containing high -dense SA, ECG, EC, L, CFA and perlite Mortar containing high -dense SA, ECG, EC, L and CFA
Mortar containing low-dense SA Mortar containing low-dense SA and CFA
Mortar containing low-dense SA and L Mortar containing low-dense SA and L
Mortar containing low-dense SA, L and CFA Mortar containing low-dense SA, L and ECG
Mortar containing SF Newspaper sandwiched aerated lightweight concrete panels
Normal concrete Normal mortar
Normal paste Paste containing fibers and M
Paste containing fibers, SF and M Paste containing latex
Paste containing M Paste containing SF
Paste containing SF and M Paste containing SF and silane
Paste containing SF, M and defoamer Paste containing SF, M, and dichromate-treated fibers
Paste containing SF, M, defoamer and O3-treated fibers Paste containing SF, M, defoamer and silane-treated fibers
Paste containing SF, M, defoamer and as-received fibers Paste containing SF, M, defoamer and dichromate-treated fibers
Paste containing SF, M, defoamer and O3-treated fibers Polystyrene foamed concrete
Steel fiber concrete Steel fiber concrete with high fiber concentration
Expon. (ACI committee 213 R-03) Expon. (Thermal conductivity )

4.0

3.5

3.0
Thermal conductivity, k (W/m °K)

2.5

2.0

1.5 ACI committee 213 R-03

y = 0.0864e0.0013x

1.0

y = 0.05e0.00x
R² = 0.80
0.5

0.0
0 500 1000 1500 2000 2500 3000

Dry density, ρ (kg/m3)

1395

1396 Figure 18 - Density and thermal conductivity of cement-based materials

59
1397 (i) Normal concrete [1631, 2032-2035], newspaper sandwiched aerated lightweight concrete panels
1398 [2036], polystyrene foamed concrete [2037], alkali-activated concrete based FA and oil palm shell
1399 [2038], concrete containing FA [1956, 1958], SF [1956, 1958], SF and GGBS [1958], SF and FA [1958],
1400 GGBS [1958], FA and GGBS [1958], CNT [1631], lightweight aggregates - LWA/Argex [1022], LWA/ex-
1401 panded clay (EC) [2036], LWA/expanded shale [2036], LWA/Leca [1022], LWA/Lytag [1022], LWA/pum-
1402 ice [2034], LWA/Stalite [1022], RHA [2035], silane and SF [1957], wood-based aggregate [2033], brass
1403 shavings [2032], copper wires [2032], micro PCM [2032], PCM dispersion [2032], PCM pellets [2032],
1404 foamed concrete [2039], graphite and magnetite [2032], graphite [2032], and steel fibres [2032];

1405 (ii) Normal mortar [2040], mortar containing FA [2041], SF [2041], GGBS [2041], EC [2042], expanded
1406 cork granules (ECG) [2042], High-dense SA and EC [2042], high-density SA, ECG, EC, lime (L) and FA
1407 [2042], high-density SA, ECG, EC, L, FA and perlite [2042], high-density SA, ECG, EC, L and FA [2042],
1408 low-density SA [2042], low-density SA and FA [2042], low-density SA and L [2042], low-density SA, L
1409 and FA [2042], low-density SA, L and ECG [2042];

1410 (iii) Normal paste [2032, 2040, 2043], paste containing fibres and methylcellulose (M) [2043], fibres,
1411 SF and M [2043], latex [2043], M [2043], SF [1957, 2043], SF and M [2043], SF and silane [2043], SF, M
1412 and defoamer [2044], SF, M, and dichromate-treated fibres [2044], SF, M, and silane-treated fibres
1413 [2044], SF, M, defoamer and O3-treated fibres [2044], SF, M, defoamer and silane-treated fibres
1414 [2044], SF, M, defoamer and as-received fibres [2044], SF, M, defoamer and as-received fibres [2044],
1415 SF, M, defoamer and dichromate-treated fibres [2044], SF, M, defoamer and O3-treated fibres [2044].

1416 14 Summary

1417 The aim of this study is to collect and organize the main sustainability strategies considered to offset
1418 the negative impact of CBM’ production. Thus, the strategies are divided in 12 sections. In each one,
1419 a number of sub-strategies, future trends and their limitations are presented. Thus, the outputs of the
1420 main sections are briefly presented in the following paragraphs:

1421  Reduce the total amount of binder. Despite few studies on concrete with low binder content,
1422 the results of the literature show that, in opposition to the limitations imposed by standards,
1423 concrete with an acceptable performance can be produced by following the strategies men-
1424 tioned in this paper such as using a w/b in which most the water content is absorbed by the
1425 hydration products (additional water is the main contributor to porosity);

1426  Reduce the EI and resources use of binders. Most of the strategies that decrease the EI and

60
1427 resources use of binders are related to replacing cement with by-products. Despite many case
1428 studies, this strategy may not be one of the best to decrease the EI of concrete, but it is still
1429 the most popular one because it is easy to perform. According to many studies, the biggest
1430 challenge on the use of many by-products in concrete structures is durability, namely in terms
1431 of carbonation (the mechanical characteristics of the concrete cross-sections can be compro-
1432 mised because of reinforcement corrosion). Nevertheless, this output resulted from labora-
1433 tory tests (accelerated carbonation) that may not correctly reproduce reality. For example,
1434 some studies show that, even when carbonation resistance is designed for XC3 and XC4 expo-
1435 sure classes, concrete with common cover depth can protect rebars for more than 50 years
1436 even when using varying volumes of by-products;

1437  Reduce the EI and resources use of aggregates. Even though the consumption of natural ag-
1438 gregate is 12 times higher than that of cement, its EI relatively to cement is inconsequential.
1439 Nevertheless, the EI of aggregate production is still growing at an alarming rate compared to
1440 the capacity of Nature. This study shows that, besides natural aggregates and construction
1441 and demolition waste, there are many other potential sources (e.g. agricultural, industrial,
1442 municipal wastes) of aggregates in concrete. In most cases, aggregate’s content and charac-
1443 teristics do not affect the durability of CBM (the main factor to define service life) as much as
1444 those of binders. However, the applicability of most non-traditional aggregates depends on
1445 the target-strength of concrete and the influence level varies a lot. Thus, many of the non-
1446 traditional aggregates have been recommended to be used in low-strength concrete only;

1447  Increase the durability of reinforced concrete. The biggest challenge of this strategy is the fact
1448 that normally the initial cost increases. However, it may also considerably reduce costs over the
1449 structure’s life cycle (long-term) because the number of rehabilitations necessary in low-perfor-
1450 mance concrete is higher than in high-performance concrete (also taking into account the very
1451 important role of the reinforcement concerning this issue). Thus, the total cost of low- perfor-
1452 mance concrete will get closer to that of high-performance concrete with every rehabilitation;

1453  CO2 mineralization and utilization (carbon capture and storage). Low-carbon to near-zero-
1454 carbon cements is not possible without CO2 capture by mineralization of CBM. This study
1455 shows that, apart from Mg, there are many other techniques and other potential metals that
1456 can capture high amounts of CO2.

1457  Thermal conductivity improvement and energy saving. This analysis show that, regardless of
1458 the type of used materials (traditional or non-traditional), it can be said that density is the

61
1459 major parameter to determine the thermal conductivity of any type of CBM. Nevertheless,
1460 there is not a systematic study to suggest an optimum material among all the non-traditional
1461 materials in terms of thermal conductivity and quality of the CBM.

1462  Material manufacturing. This study shows that it is not possible to significantly decrease the
1463 EI and resources use of concrete without considering the production stage of the raw materi-
1464 als. Nevertheless, studies on this path for most of the materials are very scarce.

1465 As shown in Figure 19, the following statements can be made about most of the selected strategies.
1466 Most of the researchers are mainly focused on the same common non-traditional techniques and mate-
1467 rials (e.g. FA, SF, GGBS and RHA) with similar output. Nonetheless, there are many other non-traditional
1468 techniques and materials (e.g. low binder concrete; using many types of AWAF and municipal wastes as
1469 a binder or aggregates; nonconventional bars, production process of the main products by using differ-
1470 ent types of raw materials and energy; new site applications) that have not been investigated yet. The
1471 analysis also shows that there is a big scatter in characteristics of the uncommon non-traditional mate-
1472 rials. Thus, they need to be classified in different categories in order to be used in CBM.

Many studies Few studies Rare studies

Traditional materials Cost/economy

Common non-traditional materials Environmental impact and resource use

Uncommon non-traditional materials Quality/technical characteristics

All above All above

1473

1474 Figure 19 - The predominant flows of previous studies (Right side - uncommon non-traditional materials and all above 
1475 left side - all above, no study found)

1476 In conclusion, for the same non-traditional materials and techniques, many studies have been focused
1477 on few characteristics, ignoring most of the others. Thus, conclusions identifying a sustainable mate-
1478 rial or technique based on one aspect only (e.g. environmental impact, quality or costs) may not be
1479 reliable. For example, some strategies may decrease the CBM’s EI. However, the strategy may de-
1480 crease the CBM’s durability performance and therefore reduce its service life. Thus, buildings may
1481 require further rehabilitation to obtain a target service life. Similar reasoning could be stated for costs,
1482 which is the most important parameter considered in business as decision-making. Thus, adequate
1483 strategies can only be defined using a holistic approach, in which all the previous aspects are taken
1484 into account.
62
1485 15 Acknowledgments

1486 The authors would like to acknowledge the support of CERIS unit from IST-University of Lisbon and
1487 the Foundation for Science and Technology of Portugal. The careful revision of the manuscript by Dr
1488 Rui Silva is also acknowledged.

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