CHEMISTRY & CHEMICAL TECHNOLOGY

Vol. 10, No. 4(s), 2016 Chemical Technology

Serhiy Pyshyev, Volodymyr Gunka, Yuriy Grytsenko and Michael Bratychak

POLYMER MODIFIED BITUMEN: REVIEW

Lviv Polytechnic National University
12, S. Bandery St., 79013 Lviv, Ukraine
Received: September 02, 2016 / Revised: September 22, 2016 / Accepted: October 01, 2016

 Pysh’yev S., Gunka V., Grytsenko Yu., Bratychak M., 2016

Abstract. The main reasons and ways of bitumen The largest importers of bitumen are [3]: China –
modification by polymers were examined. Positive and 3.225 mln.tons (19.8 %); USA – 1.641 (9.8); France –
negative aspects of the usage of different polymer 1.193 (7.1); Saudi Arabia – 0.996 (5.9); Algeria – 0.729
modifiers (elastomers, thermoplastic elastomers, reactive (4.3). Ukraine imports 0.165 mln.tons (1.0 %; 21st place in
polymers, thermoplastics) were analysed. The authors’ the world).
achievements concerning modification of bitumen by World consumption of bitumen is on the average
various polymers, namely indene-coumarone, petroleum, 87 mln.tons per year [5]. The structure of consumption by
phenol-formaldehyde and epoxy resins, were described. world regions is shown in Fig. 1.
About 85 % of petroleum bitumen are used as a
Keywords: polymer modified bitumen, elastomer, binder in various types of asphalt laying: sidewalks,
thermoplastic elastomer, reactive polymer, thermoplastic. highways, airports, etc. [4, 5] (Fig. 1).
To date bitumen-mineral mixtures for pavement are
prepared by two ways: (i) as a result of bitumen heating to
1. Introduction the temperatures exceeding their dropping points; (ii) by
obtaining aqueous bituminous emulsions. Table 1
According to [1] in 2013 ten major bitumen represents the composition of petroleum bitumen
producers are: USA – 19.365 mln.tons (18.9 %); China – consumption by the road industry in Europe according to
17.938 (17.5); Russia – 6.193 (6.0); India – 6.193 (4.7); EAPA (European Asphalt Pavement Association) [6].
Canada – 4.335 (4.2); Iran – 3.896 (3.8); Japan – 3.659 When using bitumen for the production of asphalt
(3.6); South Korea – 3.614 (3.5); Germany – 3.410 (3.3); mixtures it is not always possible to create a material that
Italy – 3.104 (3.0). These countries account for 68.5 % of fully satisfied consumers by their performance properties.
world bitumen production. Ukraine occupies only 53 In particular, bitumen is generally characterized by poor
place – 0.123 mln.tons (0.1 %). adhesion, low temperature and plastic properties, leading to
The largest exporters of bitumen are [2]: South poor strength of the roadway. One of the ways of solving
Korea – 2.264 mln.tons (11.5 %); Iran – 2.179 (11.1); this problem is modification of commercial bitumen.
Singapore – 2.178 (11.1); Canada – 1.778 (9.0); USA – Modified bitumen is characterized by improved flexibility
1.539 (7.8). Due to the deficit Ukraine actualy does not and longer service life, it also has a lower brittleness
export bitumen. temperature and higher softening temperature [7-10].

Fig. 1. World consumption of bitumen

632 Polymer Modified Bitumen: Review

Table 1
Consumption of bitumen in the road industry [6]
Tonnage in 2014, Percent of modified bitumen (of total) Emulsions in
Country
mln. t in 2011 in 2012 in 2013 in 2014 2014, mln. t
Austria 0.37 25.0 25.0 30.0 18.9 0.005
Belgium 0.21 25.5 27.0 25.4 26.5 No data
Croatia 0.13 No data No data No data 10.00 No data
Czech Republic 0.33 18.0 22.4 22.1 21.5 0.008
Denmark 0.19 5.0 5.0 5.0 5.0 0.020
Estonia 0.08 No data No data 4.0 3.3 0.016
Finland 0.27 0 No data 0 0 0.001
France 2.47 <10 13.0 13.0 6.9 0.792
Germany 1.60 No data No data No data No data No data
Great Britain 1.28 8.0 8.0 8.0 8.0 0.100
Greece No data 2.0 1.5 2.2 No data No data
Hungary 0.19 11.0 15.4 30.0 25.0 0
Iceland No data No data No data No data 0 0
Ireland 0.13 No data No data No data No data 0
Italy No data 14.0 13.0 14.0 No data No data
Lithuania No data 14.0 11.0 No data No data No data
Luxembourg 0.05 20.0 30.0 No data 15.0 No data
Netherland 0.30 No data No data 5.0 No data No data
Norway 0.35 15.0 No data No data No data No data
Poland No data 21.0 22.0 25.0 No data No data
Romania 0.20 74.0 45.0 76.0 75.0 0
Serbia 0.26 14.7 6.0 4.2 4.4 No data
Slovakia 0.08 60.0 37.0 31.0 29.1 0
Slovenia 0.07 10.0 11.0 9.0 10.0 No data
Spain 0.56 13.1 19.6 10.0 15.0 0
Sweden 0.45 6.0 5.0 No data 7.0 0
Switzerland 0.28 10.0 11.0 2.0 12.0 0
Turkey 2.39 8.0 7.5 4.4 3.2 0.026

The share of modified bitumen, relative to its total From a technical point of view, to create a bitumen-
use in road construction, is irregularly distributed between based composite materials with a given set of properties
European countries, but as a rule, this share is above 10 %. only those substances may be applied, which meet the
The leaders are (%): Romania – 75; Slovakia – 29.1; following requirements [17]:
Belgium – 26.5; Hungary – 25; Czech – 21.5 (Table 1). • they are not destroyed at the temperature of
asphalt-concrete mixture preparation;
2. Bitumen Modification • they are compatible with bitumen during the
mixing process on conventional equipment at the
As mentioned above, due to its natural properties temperatures usual for preparation of asphalt-concrete
petroleum bitumen is not able to create the conditions for
mixtures;
long-term operation of pavement under modern heavy
duty traffic and adverse weather factors. • in summer they increase the stability of bitumen
Therefore, in addition to providing the required (which is a part of the roadway) to the deformation impact
quality and durability it is necessary to radically improve loads without increasing its viscosity at the temperatures
the physical and mechanical characteristics of these of mixing and laying and do not impart brittleness to
materials by complex modification with additives. bitumen at low temperatures;
 Serhiy Pyshyev et al. 633

• they are chemically and physically stable and do 4) thermoplastics – polyvinyl acetate, polystyrene,
not change their properties during transport, storage, polyisobutylene, polyethylene, polypropylene, atactic
processing and operating conditions of pavement. polypropylene, polyvinyl chloride, thermoplastics
Elvaloy-4170 (copolymer of ethylene with butyl acrylate
2.1. Classification of Petroleum Bitumen and glycidyl methacrylate), latexes of Butonal NS type,
Modifiers Viskoplast-S, ethylene methyl acrylate (EVA), petroleum
resins.
According to their action the modifiers can be By volumes of using the polymers are placed in the
divided into adhesion, plasticizing, structuring and following order: thermoplastic elastomers of SBS type;
complex ones. thermoplastics of ethylene vinyl acetate type (EVA),
Adhesion additives significantly improve bitumen polyisobutylene, polypropylene, a variety of block
adhesion to stone materials and, as a rule, bitumen copolymers; polymer latexes and thermopolymers of
particles with each other, provide high water resistance of ethylene glycidyl acrylate type [9, 10].
asphalt-concrete and prevent damage of the pavement.
Adhesion additives also retard the bitumen aging [11, 12]. 2.2.1. Elastomers
Plasticizing additives provide modified bitumen This type of modifiers includes polymers, rubbers
with necessary consistency due to which they withstand and rubber polymers [9, 10, 18-24]. For the bitumen-
deformation load and temperature changes [13]. polymer composition rubber imparts a new property –
Structuring additives can become cross-link flexibility, which is typical of natural rubber in a wide
binders and thereby provide the required strength of the temperature range. The new rheological state provides
roadway coating. composition deformation at low temperatures, despite the
Complex additives are widely used in the road- lack of plastic properties of bitumen. In other words, this
building. They significantly improve the rheological additive in bitumen improves its extensibility and
properties of modified bitumen and their adhesion to elasticity at low temperatures, improves thermal and crack
mineral materials surface [14-17]. resistance, strength, deformation resistance, water
Additives for improving roadway quality are resistance, frost resistance, durability, resistance to aging.
introduced into bitumen or directly into asphalt-concrete Rubber can be introduced into bitumen by direct
mixtures. fusion, or in the presence of a solvent.
Additives which are introduced directly into The example of most suitable for bitumen
bitumen can be divided into: polymer compounds, ad- modification elastomers is synthetic rubbers of general
hesive agents and specific components (e.g. sulfur). purpose (isoprene, divinyl, divinyl styrene, ethylene
Additives introduced into asphalt-concrete mixtures are propylene). These rubbers are produced as a briquetted
divided into: stabilizing (based on fibers), structuring solid elastic product which is used for gum production via
(mineral powder, cement), structuring and stabilizing rubber vulcanization.
(natural bitumen, polymers, waxes). The compounds used The main disadvantage of elastomers is their poor
to produce polymer modified bitumen (PMB) are dispersion in bitumen, so special measures are needed to
described below. obtain homogeneous modified bitumen (fusing, special
Modification by polymer materials is one of the solvents, etc.). Moreover, phase separation between
most perspective ways to improve the quality of binders to polymer and bitumen in a liquid phase takes place,
produce road surfaces with improved characteristics. especially during storage. To avoid this phenomenon
complicated devices that can support high temperatures
2.2. Polymer Modifiers and PMB continuous mixing are needed.
According to the published data [23, 24] rubber
Polymer compounds, used as modifiers, may be crumb is a promising product to be used for the
assigned to one of four groups according to their nature, modification. The main advantages are low cost and
which implies a way to influence the properties of bitumen possibility of tires and other waste rubber products
and method of introduction into PMB [7, 9, 16-17]. recycling. Despite the obvious advantages over other
1) elastomers – natural and synthetic rubber, rubber modifiers, using crumb rubber in road building is also
crumb; limited because of the technological difficulties that arise
2) thermoplastic elastomers – block copolymers of when they are mixed with bitumen.
butadiene and styrene type SBS;
2.2.2. Thermoplastic elastomers
3) thermosetting plastics – various copolymers and
kooligomers (further – resins), which are usually have a There are three types of styrene block copolymers:
large number of functional groups: epoxy, furfurol- and styrene-butadiene-styrene (SBS), styrene-isoprene-styrene
phenol-formaldehyde, carbamide, silicone, etc. (SIS), styrene-ethylene / butylene-styrene (SEBS). The
634 Polymer Modified Bitumen: Review

content of polymers in PMB can reach 3–10 wt %. The use of TP for bitumen-polymer mixtures create
Thermoplastic elastomers (TE), compared to a number of disadvantages [7]:
thermoplastics, are characterized by higher elasticity, i.e. – when entering hardener the technological
TE combine the strength of thermoplastics and elasticity properties of PMB are almost immediately deteriorated;
of elastomers [7, 9, 10, 18-20, 25-27]. – rigidity is increased at low temperatures;
Styrene block copolymers of SBS type are mostly – the use of special hardeners complicates the
used for bitumen modification due to their ability to system and raises its price;
increase the strength of bitumen, and to provide polymer- – the effectiveness of thermosetting plastics appears
bitumen compositions with elasticity, including that at low usually at their large quantities in bitumen – more than
temperatures. Thermoplastic elastomer of SBS type is a 10 wt %.
linear polymer, which provides elasticity (ability to initial
distortion) for bitumen-polymer system due to its structure 2.2.4. Thermoplastics
(styrene units are linked by butadiene "flexible" blocks). These polymer additives improve strength and
TE retain the ability to highly elastic deformations within deformation characteristics of bitumen and asphalt: the
the temperature range of 193–353 K. The temperature of resistance to rutting at elevated temperatures increases,
TE destruction is 463–483 K. risk of cracking at low temperatures and fatigue cracking
Block copolymers of butadiene and styrene of SBS of asphalt under prolonged stress is reduced. Polymers
type are well combine with bitumen because polystyrene which are quite often used now: polyvinyl acetate,
and polybutadiene are swelled in paraffin-naphthenic and polystyrene, polyisobutylene, polyethylene,
aromatic hydrocarbons of bitumen and partially dissolved polypropylene, atactic polypropylene, polypropylene,
in them at 423 K. polyvinyl chloride, Viskoplast-S, EVA, ethylene methyl
To improve polymer dissolution in bitumen the acrylate [7, 9, 10, 18, 20, 37-40]. However, the use of
plasticizers are used (usually a mixture of aromatic based "traditional" polymers (polyethylene, polypropylene, etc.)
hydrocarbons). Plasticizer significantly improves the is accompanied by a number of problems because rigidity
polymer solubility in bitumen, but slightly decreases the and brittleness of resulting PMB increase after
adhesive properties of the resulting binder compared to modification. As a result, a pavement using such binders,
the original bitumen [7, 10]. is disposed to increased cracking at low temperatures.
Due to their properties TE are produced in a variety Synthetic latex of Butonal NS type (BASF,
of trademarks [28-31]: Kraton D1101, Kraton D1184, Germany) [41-44] and thermopolymers of Elvaloy series
Kraton D1186 (Kraton Polimers, USA); Finaprene 411 (DuPont, USA) [7, 18, 45] are widely used. These
(Total, France); Europrene Sol T 161B (Eni, Italy); polymers not only reduce bitumen sensitivity to
Calprene 411 (Dynasol, Spain); DST 30-01 and DST- temperature changes, but also enhance the cohesive and
30R-01 (Voronezh factory, Russia). adhesive strength resulting in the increase of strength and
The main disadvantage, restraining the growth of crack resistance of asphalt concrete pavement.
modified bitumen production is its high cost. Bitumen Petroleum resins obtained from by-products of
modified by TE is 1.5–2.5 times more expensive than fossil fuels thermodestruction occupy a special position
unmodified bitumen [8]. among thermoplastics. They can be used to improve
bitumen properties, namely they increase the viscosity,
2.2.3. Thermosetting plastics
hardness, durability and adhesion to mineral materials
Thermosetting plastics (TP) are polymers, which [46- 48]. The additives containing polar groups in their
turn into solid state while heating or introducing hardener. molecules, contribute to improved wettability of the
Before hardening TP molecules have a linear structure, mineral materials with bitumen, creating an adsorption
the same as thermoplastics molecules, but the size of their and hemosorption monomolecular layers providing strong
molecules is significantly smaller. TP molecules are adhesion of bitumen-mineral mixture.
chemically active. They contain either double Petroleum resins with functional groups are of
(unsaturated) bonds or chemically active groups. special attention. These compounds may belong both to
Therefore, under certain conditions (at heating, irradiation thermoplastics and thermosetting plastics. The presence of
or adding hardeners) thermosetting molecules react with functional groups in petroleum resin structure
each other and form a continuous network. Epoxy, significantly improves the adhesion properties of
phenol-formaldehyde, carbamide, polyester, silicone and bituminous materials, resulting in increased durability of
other resins belong to TP [7, 9, 10, 32-36]. the products based on them. The use of petroleum resins
Bitumen-polymer binders with thermosetting for bitumen modification is limited due to their
plastics have relatively high adhesion to the mineral considerable cost. Moreover, under high temperatures
particles and high strength. these compounds can form three-dimensional cross-linked
 Serhiy Pyshyev et al. 635

structure with petroleum bitumen that reduces its the wastes obtained during haydite and soda production are
plasticity. As a result cracking of asphalt pavement added to bitumen. The use of haydite dust improves crack
occurs. Under long-term exposure to high temperatures resistance and strength characteristics of the bituminous
during preparation, transportation and laying of road binder. When using wastes of soda production the asphalt
surfaces thermal degradation of polymers is also possible, strength is quite high but water resistance after long-term
so they can lose modifying properties. water saturation is below limit. This problem may be solved
Resin modifiers may also be produced from coal by using silica powder [62]. However, mineral fillers do not
processing secondary products. The investigations usually improve adhesion and/or plasticity of bitumen.
concerning using indene-coumarone resin (ISR) as a
modifier were carried out at the Department of Oil and
Gas Processing of Lviv Polytechnic National University 3. Conclusions
[49-51]. ISR is a polymerization product of a mixture of
compounds (mainly indene, coumarone and styrene), 85 % of bitumen production (on the average about
which are by-products of the coking process ("heavy" 90 mln.tons of bitumen per year) is used as a binder in
benzene, coal tar light fractions). ISR introduction into road construction. However oxidized and residual bitumen
bitumen significantly increases its softening temperature does not have the necessary properties to meet modern
(from 320 to 325 K) and significantly improves the requirements to the pavement.
adhesion properties (Table 2). On the other hand, the The most common way to increase the
plastic properties of bitumen are deteriorated (penetration performance properties of oil bitumen (primarily, oxidized
and ductility decrease), the same as while using other bitumen) is the use of various polymers as modifiers.
thermoplastics and majority of thermosetting plastics. Polymer modified bitumen compared to conventional
Therefore, as a plasticizer it is proposed to use tar and/or bitumen has a number of significant advantages. They are
resin, which is a by-product of brown coal oxidative more elastic, flexible and durable, less sensitive to the
desulphurisation [52-57]. temperature changes and aging, have better adhesive and
cohesive properties.
2.3. Non-Polymer Modifiers Thermoplastic elastomers, particularly SBS, are
most widely used as bitumen modifiers due to their
Other types of modifiers (non-polymer modifiers) complex action. They provide bitumen with high strength
should be mentioned here, as well. Sulfur is considered to (the same as thermoplastics and thermosetting plastics),
be the most promising among them. Technical sulfur is elasticity (as elastomers), heat resistance, adhesion, and
inexpensive and small-scale product. While producing improved low-temperature characteristics. But the main
sulphur asphalt the part of expensive bitumen is reason that restrains thermoplastic elastomers prevalence is
substituted for relatively cheap sulfur (50 wt %). The their high cost. An effective solution of this problem is their
result is reduction of the finished product price and partial or complete replacement by cheaper polymers.
improvement of asphalt properties. Sulfur asphalt has A promising direction is the production of
several unique properties such as high compressive and modifiers from by-products of fossil fuels thermo-
flexural strength, adhesion, chemical resistance, frost destruction, which contain a sufficiently large amount of
resistance, low water absorption and waterproofness. A unsaturated compounds. Among mentioned by-proucts are
major disadvantage of sulfur compositions is their low "heavy" benzene and/or coal tar light fractions, obtained at
thermal stability. In addition, there is a significant change coke plants and used for the production of indene-
in volume during sulfur solidification due to phase coumarone resin. The latter one can be used to produce
transition of sulfur from a liquid to a solid state [58-61]. modified bitumen, which meets regulatory requirements
Mineral materials are often added to bitumen but and has extremely high adhesion (till 100 %).
they should be rather fillers than modifiers. For example,
Table 2
ICR modified bitumen
Blend composition, wt % Main characteristics of resulting PMB
Plasticizer Softening temperature Ductility at Penetration at Adhesion to
bitumen IСR plasticizer
(ball & ring method), K 298 K, m·10-2 298 K, m·10-4 glass, %
– 100.0 0 0 320 75 62 46
– 93.0 7.0 0 325 36 38 100
Resin of brown coal
84.0 7.0 9.0 325 28 62 100
thermodestruction
Tar produced from West-
85.0 7.0 8.0 325 26 60 93
Ukrainian oils [52-57]
636 Polymer Modified Bitumen: Review

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