C. R.

Chimie xxx (2018) 1e13

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Low-cost ceramic membranes: Synthesis, classifications, and

applications
Mansour Issaoui a, b, *, Lionel Limousy c
a
University of Sfax, National School of Engineers, Laboratory of Industrial Chemistry BP1173, Sfax, Tunisia
b
Wastewaters and Environment Laboratory, Water Research and Technologies Center, P.O. Box 273, Soliman 8020, Tunisia
c
University of Strasbourg, University of Haute-Alsace, Institute of Materials Science of Mulhouse (IS2M e UMR CNRS 7361), Mulhouse,
France

a r t i c l e i n f o a b s t r a c t

Article history: The elaboration of porous ceramic membranes using low-cost materials has attracted
Received 24 June 2018 much interest. Indeed, the choice of suitable raw materials (including additives or binders)
Accepted 21 September 2018 is critical to the membrane's performance. However, with the growing need for more cost-
Available online xxxx
effective resources with superior performance, many studies have been conducted for
selecting suitable cheap raw materials for the intended use and then adjusting the overall
Keywords:
characteristics, and therefore allowing the ceramic membranes to be tailored to suit a wide
Ceramic membranes
range of industrial applications. Many attempts have been made by researchers to produce
Membrane production
porous ceramic membranes from specific materials, but their industrial applications
Membrane applications
remain very limited because of the high cost of the raw materials used. The use of ceramic
Membrane technology
materials for producing membranes has many advantages, such as high mechanical and
chemical stability and excellent thermal resistivity. The evaluation of membrane perfor-
mances, essentially their permeability and rejection, can assert their use in many industrial
fields, namely beverage and food, pharmaceutical, biotechnology, petrochemical industries
as well as water treatment and several other environmental problems. This article aims to
make a thorough review of the different processes used in the synthesis of ceramic
membranes using inexpensive raw materials as well as their intrinsic characteristics and
industrial applications in several sensitive fields taking into account both economic and
environmental aspects.
© 2018 Académie des sciences. Published by Elsevier Masson SAS. All rights reserved.

1. Introduction through the membrane is called the permeate, whereas the

retentate is the liquid consisting of the retained elements.
A membrane can be defined as a selective partition, Generally, a ceramic membrane has an asymmetrical
which under the effect of a driving force will permit or structure composed of three layers (Fig. 1): The outer layer
prevent the flow of certain elements between the two forms a macroporous support and provides a high me-
media it separates. A transfer force may be generated by a chanical strength for the fabricated membrane. The second
gradient of pressure, concentration, or electrical potential layer is the inner layer ensuring the separation. The inter-
applied to induce the permeation through the membrane. mediate layer binds the inner and the outer layers [2].
In most cases, the membrane module consists of an inlet Nowadays, the use of membrane separation processes
(feed) and two outlets. The part of the fluid that passes has become more important in many industrial applica-
tions, especially as they have been proven to be highly
efficient in many separation processes, including industrial
* Corresponding author. effluent water treatment [3,4], air purification, food
E-mail address: issaouimansour@yahoo.fr (M. Issaoui).

https://doi.org/10.1016/j.crci.2018.09.014
1631-0748/© 2018 Académie des sciences. Published by Elsevier Masson SAS. All rights reserved.

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2 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13

2. Manufacturing of ceramic membranes

Elaboration of ceramic membranes can be carried out in

three steps: the first step consists in the formation of par-
ticle suspension, the second step consists in shaping the
particle suspension into a membrane precursor with a
desired geometry, and the final step consists in heating the
membrane precursor [2]. The obtained substrate can be
modified by the layer deposition method tailoring the
membrane selectivity and other membrane properties.
Ceramic membrane supports can be fabricated using
different methods depending on the application re-
quirements, the desired membrane structure, and the
Fig. 1. Schematic diagram of a composite membrane: (A) top layer, (B) in- specific materials. The most common manufacturing pro-
termediate layer, and (C) porous support [1]. cesses are slip casting, tape casting, pressing, extrusion, and
freeze casting [27,28].

industries, and other environmental applications [5,6]. The 2.1. Slip casting method
research on new membrane technology would allow using
a membrane process for solving many environmental Slip casting is a simple and economical technique oc-
problems at low cost. casionally used for advanced ceramic membrane prepara-
Among the most commonly used materials for the tion. This method has been used for a long time in the
manufacture of ceramic membranes we quote alumina traditional ceramic industry [29]. This method has the ad-
(Al2O3), zirconia (ZrO2), titania (TiO2), silicon carbide (SiC), vantages of shaping complex geometries and irregular
glass (SiO2), or a combination of these metal oxides, and forms and also achieving good material homogeneity.
other suitable materials including nonoxides (carbides, ni- Indeed, a particle suspension is well mixed and then
trides, borides, and silicides) and composites of combina- poured into a porous mold, so that the solvents can diffuse
tions of oxides and nonoxides, as well as other clay minerals through the pores because of the driving capillary action,
(e.g., kaolin, mullite, dolomite, etc.). Ceramic membranes forming a cake layer by particle precipitation on the internal
are thermally stable, possess excellent tolerance to pH, and surface of the mold, followed by a rapid consolidation step of
can withstand temperatures of up to several hundred de- the particle layer to avoid particle penetration through the
grees Fahrenheit. mold (Fig. 2) [30]. This method has been applied to prepare a
In fact, remain challenge from the cost benefit point of ceramic membrane from different low-cost materials, such
view, the optimization of membrane filtration perfor- as kaolin [31] and fly ash [22,32]. Generally, ceramic mem-
mance. For this reason, porous ceramic membranes have branes prepared by slip casting are known for their high
been used extensively in many industrial processes because permeation properties, resulting in the presence of smaller
of their many well-known advantages as compared with pore size over thinner region. Jedidi et al. [22] have reported
polymeric membranes [7e9]. Thus, many commercialized the use of the slip casting method for developing a porous
ceramic membranes have been made from expensive tubular ceramic membrane based on mineral coal fly ash. The
compounds, such as cordierite [7,10], titania, zirconia obtained membrane has a homogeneous surface without any
[11,12], and silicon carbide [13]. macrodefect when heated at 800
C, having an average pore
Recently, to reduce the cost of membranes researchers diameter of about 0.25 mm and a hydraulic permeability of
have focused their attention on the production of ceramic about 475 L/(h m2 bar). The obtained membrane was applied
membranes using cheap raw materials, such as natural clay in the treatment of dyes from wastewater generated by the
[14], apatite powder [15], dolomite, kaolin, bauxite wash baths in the textile industry.
[16e20], and mineral coal fly ash [21,22].
The preparation of a porous ceramic membrane with 2.2. Tape casting method
enhanced porousness and effective separation presents a
great interest. Several researches used several pore- Tape casting method is a widely used fabrication tech-
forming agents such as aluminum powder [19], sawdust, nique in the production of thin and smooth ceramic sheets.
starch, carbon, or organic particulates [23e25]. This technique, which was introduced by Glen N Howatt in
Ceramic membranes are the most used in the industrial the mid-1940s during the Second World War for the pro-
field. They are not easy subjects to bacterial contamination duction of thin piezoelectric materials [33], has been
and abrasion as organic membranes [26]. Furthermore, they known for a long time for the production of ceramic
can preserve their flow and water permeability properties membranes. This technique involves pouring the powder
over time. suspension into a reservoir, which in turn passes under an
This article outlines an extensive overview of research adjustable casting knife that controls the thickness of the
projects in the preparation of low-cost porous ceramic cast layer, defined by the gap between the knife blade and
membranes with high performances, used as filters in the moving carrier. After that, the ceramic tape obtained
many different industrial processes and also for solving passes through a drying zone where solvent evaporation
various environmental problems. from the membrane surface takes place (Fig. 3) [34].

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 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13 3

Filling Casting Emptying Resulting cast

Fig. 2. The principle of slip casting method to prepare ceramic membranes [30].

This method has been adopted by several researches for of a dry powder by means of a press machine. Indeed, after
the fabrication of a ceramic membrane [1,9,35]. Nandi et al. mixing the powder homogeneously (raw material with
[36] have elaborated circular discs of 52.5 mm diameter pore-forming agent ratios), the obtained product is pressed
and 4.5 mm thickness from kaolin and other suitable low- uniaxially (Fig. 4), that is, it undergoes stress by a punch in a
cost materials such as quartz, calcium carbonate, sodium mold with immobile walls to obtain the desired membrane
carbonate, sodium metasilicate, and boric acid. After sin- support shape. This process allows very high production
tering at 1000
C, the obtained ceramic membrane has rates. For consolidation, the obtained flat membrane sup-
good properties with an average pore size, porosity, and port must go through heat treatment, generally at a tem-
flexural strength of 810 nm, 33%, and 8 MPa, respectively. perature reaching that of the used materials sintering [38].
Also, Jana et al. [37] have studied the use of clay and kaolin Generally, ceramic membranes produced by the press-
mixture to prepare a low-cost ceramic membrane by tape ing method have well-defined characteristics, such as
casting method, the obtained ceramic discs sintered at uniform porosity and homogeneous physical properties
1000
C have shown good performances, with an average over the total membrane part. Del Colle et al. [39] have
pore size, porosity, pore density, and flexural strength of applied this method to manufacture tubular porous and
0.31 mm, 22%, 4.80  1012 m2, and 12.81 MPa, respectively. supported ceramic membranes based on zirconia. The
Das et al. [35] have also synthesized an alumina membrane microfiltration (MF) porous membranes exhibit an average
by the tape casting method, with pore size and porosity pore size of 1.8 mm, whereas the ultrafiltration (UF) ones
ranging from 0.1 to 0.7 mm and 25e55%, respectively. The present an average pores size of 0.01e0.03 mm in the top
obtained membrane has been found to be suitable for the layer and 1.8 mm in the support. The obtained ceramic
complete removal of bacteria from water. membranes were intended for the demulsification of
oilewater suspension. Hristov et al. [40] have also prepared
2.3. Pressing method low-cost ceramic membrane support by semidry pressing
of natural zeolite powder. The discs with diameter 30 mm
Pressing method is a well-known method used mainly and thickness 4 mm formed after firing at different tem-
for the fabrication of ceramic membranes for fundamental peratures (from 800 to 1000
C) presented high porosity
research. This method is commonly based on the pressing (38%) and very uniform pore distribution. In another study,

Adjustable Knife
Reservoir

Solvent Warm air source

evaporation
Gup Ceramic tape
Carrier foil Slurry

Tape casting direction

Supply Roller Collection Roller

Fig. 3. The principle of tape casting.

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4 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13

Upper Punch Pressure

Upper Punch

Raw
ceramic
Powder
Ceramic membrane

Lower Punch LowerPunch

Lower Punch

Fig. 4. The principle of pressing method.

Huang et al. [41] have introduced the pressing method at kaolin and calcite mixtures using the extrusion method.
25 MPa for producing the low-cost ceramic membrane These supports sintered at 1150
C with homogeneous
based on kaolin. Likewise, Issaoui et al. [19] have used the surfaces and interesting characteristics (an average pore
dry pressing method at 66 MPa for producing flat ceramic size of about 4 mm, a porosity ratio around 50.5%, and a
membranes from kaolin and cermet membrane supports tensile strength z28 MPa) were selected to be substrates
from kaolinealuminum powder. for the membrane layers used in MF.
Also in the same frame, recently Issaoui et al. [47] have
manufactured low-cost tubular macroporous supports for
2.4. Extrusion
ceramic membranes using the extrusion method. After sin-
tering at 1250
C, the water permeability measured was
Extrusion is also a conventional method for producing
about 612 L/(h m2 bar) for samples elaborated from a pow-
ceramic membranes, extensively used for the fabrication of
der mixture containing 80 wt% kaolin and 20 wt% of starch.
porous tubular configuration. In this method, a plasticizing
agent and binding agent are necessary for the production of
a ceramic pulp with rheological characteristics (plasticity, 2.5. Freeze-casting method
hardening degree after drying, etc.) to make shape by
extrusion possible [42]. The shaping method of the paste The freeze-casting method also called ice-templating is
depends on the geometry of the final membrane support. It considered as one of the most recent, attractive, and novel
is a plastic continuous deformation process, in which paste is technique for the preparation of highly porous ceramic
forced with a relatively simple piston press to flow through membrane structures that are hierarchically organized. In
the die opening of a smaller cross-sectional area, which this method, ceramic slurry is generally frozen by the
dictates the shape, pore size distribution, and the porosity of bottom and followed by sublimation of the frozen solvent
the final product (Fig. 5) [43]. The raw ceramic membranes under reduced temperature and pressure. Then, following a
are dried (at room temperature) and then treated under repetitive pattern the freezing of the ceramic slurry results
high-temperature conditions, generally at a low ramping in the growth of upright solvent crystals along the freezing
rate to avoid the formation of cracks on the ceramic layer, up direction and the related rejection of ceramic particles
to the sintering temperature of the used material. The between these crystals (Fig. 6).
extrusion process has been commonly used to prepare At the end of these steps, the obtained porous raw
different ceramic membranes using inexpensive materials. membranes showed a main shortcoming that lies in their
Jedidi et al. [44] have fabricated low-cost tubular ceramic low mechanical properties. To overcome this defect, a
support for the membrane by extrusion of fly ash paste. The thermal treatment is required at the vicinity of the sinter-
obtained samples sintered at 1125
C have shown homoge- ing temperature of the used material, during which the
neous surface exempt of macrodefect, with mean pore porous structure acquires its consolidation and its walls are
diameter and the pore volume of 4.5 mm and 51%, respec- densified [48]. This technique allows elaborating ceramic
tively. Elmoudden et al. [45] have manufactured also porous membrane that can be used in very promising applications
tubular ceramic membranes from calcinated clay using the such as the generation of energy [49].
extrusion method. The sintered membranes at 1130
C have An interesting work has been performed by Liu et al. [50].
shown a mean pore diameter of 9 mm and porosity of 38%. They have used the freeze-casting technique to manufac-
Also in other studies, Boudaira et al. [46] have elabo- ture porous alumina UF membranes with good performance
rated tubular ceramic supports for membranes from local for anionic dye separation. After calcination at 1150
C, the

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 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13 5

Ceramic
powder
Water
Additives

Chamber Die

Piston Paste
Mixing

Extrudes

Drying, debending and thermal

consolidation
Fig. 5. The principle of extrusion method.

elaborated freeze-cast membrane yielded a porous struc- size, and solids loading. Tubular porous mullite supports with
ture of about 33 nm and bending strength of 36.5 MPa. Also, pore channel size of 6.5 mm, porosity of 59.66%, and
the membrane exhibits high rejection rate of 99.6% toward compressive strength of 54.11 MPa were obtained when the
Direct Red 80 solutions with permeate flux (PF) of about freezing temperature, average particle size, and solids
6.39  105 m3/(m2 s) at applied pressure of 2 bars. loading was 100
C, 2.8 mm, and 35 vol%, respectively.
Another study that introduces the freeze-casting method
was conducted by Liu et al. [51]. They have fabricated tubular 3. Membrane classifications
porous mullite membrane supports, with gradient unidirec-
tional aligned pores. The results show that the characteristics The most popular classifications of a membrane are
of the ceramic membrane supports can be adjusted by con- based on their morphology, geometry, chemical nature, and
trolling the freezing temperature, mullite powder particle separation regime [52].

Mechanical Ceramic
particles in the slurry
Freezing direction

Direction Ceramic
particles rejected
Solvent
Crystal

between growing ice

crystals

Fig. 6. Ice crystals growth during the freezing phase and the related distribution of ceramic particles excluded between the ice crystals.

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6 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13

3.1. Classification according to morphology al. [55] who have developed a tubular asymmetric UF
membrane from kaolin, exhibiting average pore sizes
We could distinguish two types of membranes according of about 1 mm and 11 nm for the support and the active
to the structures of the different construction materials: layer, respectively, with hydraulic permeability value of
78 L/(h m2 bar). In another study, Hubadillah et al. [56]
1. Symmetric (isotropic) membranes: they are dense or have prepared low-cost flat ceramic supports from
porous, and generally refer to the membrane having a kaolin, with pore size ranging from 0.38 to 1.05 mm,
relatively uniform pore size with a homogeneous porosity of 27.7%, and mechanical strength of 98.9 MPa.
structure throughout the entire thickness (Fig. 7a) [53]. - Composite membranes or skinned membranes are
Several researchers focused their attention on the those formed by deposition of thin film with necessary
preparation of isotropic membranes. For example, characteristics onto another porous film that usually
Issaoui et al. [19] have fabricated symmetric flat cermet acts as a support [57]. They also have an active layer on
supports for membranes from a mixture of kaolin and the side of the membrane with much smaller pores than
aluminum, with open porosity reaching 28.5%. Likewise, the rest of the membrane (Fig. 7b). Among the recent
Zhang et al. [54] have produced a thin tubular isotropic publications, Almandoz et al. [58] have fabricated
membrane from ceramic powder with mechanical tubular composite membranes from natural alumino-
strength of 122 MPa after sintering at 1200
C. silicates (clay, feldspar, quartz, bentonite, and alumina)
2. Asymmetric (anisotropic) membranes that present a by depositing a thin active layer on the support. After
pore size gradation decreasing toward the surface. This sintering at 1200
C, the composite membranes showed
type can also be divided into two subgroups: good structural characteristics, hydraulic permeabilities
- Membranes prepared from the same material exhibit between 10 and 274 L/(h m2 kPa), porosities close to
gradation of the pore size from one side to another. 50%, and pore diameter ranging from 0.08 to 0.55 mm for
Among recent work on this type, we can quote Rekik et the filtration layer.

Fig. 7. Symmetric (a) and asymmetric (b) membranes.

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 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13 7

3.2. Classification according to the membrane geometry tolerance to pH and high resistance to chemical degrada-
tion. Table 1 summarizes a comparison between organic
Ceramic membranes can be categorized according to and inorganic membranes in terms of their material char-
their geometry into two main groups: first, flat sheet acteristics, advantages, and disadvantages.
membranes, which are used in the construction of flat
sheet, disc, spirally wound, plate, and frame modules. 4. Critical industrial applications of ceramic
Second, cylindrical membranes, which are used in cylin- membranes
drical fiber modules. On the basis of the dimensional dif-
ferences, the following types of cylindrical membranes may Over the past few years, membrane technology has
be distinguished [59]: gained grounds and found wide-ranging applications
across a whole range of industries. Ceramic membrane
 Tubular membranes with an internal diameter larger systems are not only chosen as a filter but for other capa-
than 10 mm. bilities, namely their broader ability to coagulate, precipi-
 Capillary membranes with an internal diameter be- tate, or oxidize and eliminate chemicals. For this reason,
tween 0.5 and 10 mm. specific applications and developments have fueled its
 Hollow fiber membranes with a diameter smaller than growth and provided the seeds for subsequent opportu-
0.5 mm. nities. The first large-scale commercial success of porous
ceramic membranes has been applied in the food and
beverage industries [62e64]. However, different areas such
3.3. Classification of membranes according to the separation as biotechnology, pharmaceutical, petrochemical, water
mechanism treatment industries, environmental problem, and many
more industrial applications have been reported in the
Membrane separation processes are dependent on the literature [65,66]. The following sections provide more in-
size of the separated element and separation mechanisms. formation on the possible areas of ceramic membrane
Generally, there are three membrane separation mecha- applications.
nisms [60]:
4.1. Food processing industry
 Sieving effect mechanism: a very similar phenomenon
occurring in the normal filters. This mechanism sepa- Membrane processes are used to replace conventional
ration is based on the difference in the particle size, processing methods. They can be considered as innovative
meaning the pore size of the membrane should be methods for the production of requisite ingredients for the
smaller than the particle size, which is to be separated. new food product development or their improvement [67].
Expressions like macrospores, mesopores, and micro- Generally porous ceramic membranes based on mem-
pores are used to describe the pore size in the mem- brane processes driven by pressure namely MF, UF, NF, and
brane for MF, UF, and nanofiltration (NF). RO have been widely used. Two main classes of applications
 Solution diffusion mechanism: this is related to the can be distinguished: clarification and concentration of
difference in solubility or diffusion coefficient of each suspended particles, molecules, and microorganisms from
component in the membrane, this principle is used in
operations like reverse osmosis (RO) and requires a
dense membrane. Table 1
 Electrochemical mechanism: this is based on the dif- Comparison between organic and inorganic membranes [61].
ference in the charges of the mixture components to be Properties Organic membranes Inorganic membranes
separated. Generally, nonporous ion-exchange mem-
Material Rubbery or glassy type Inorganic materials, i.e.,
branes are used in operations like electrodialysis.
membranes based on the glass, ceramic, silica, etc.
operating temperature
Characteristic Rigid in glassy form and Chemically and thermally
3.4. Classification according to the chemical nature flexible in rubbery state stable, mechanically
robust, operational under
Membranes are classified according to their chemical harsh feed condition
nature, that is, organic, inorganic, and organic/inorganic hy- Advantages Cost-effectiveness, good Withstand harsh chemical
selectivity, easy cleaning, ability to be
brids. Organic membranes made from polymers such as processability sterilized and autoclaved,
polyamide and polysulfone derived from cellulose have been high temperature (up to
known for a long time. These membranes are not stable at 500
C), and wear
high temperature and are sensitive to oxidizing agents [60]. resistance, well-defined
and stable pore structure,
However, they may undergo sterilization with steam without
high chemical stability,
altering their structure. long life time
For the inorganic membranes, they are composed Disadvantages Fouling, chemically Fragile, rigid
entirely of mineral materials (ceramic, glass, silica, etc). nonresistant, limited
These types of membranes present several advantages, for operating temperature
and pressure, short life
instance, they are much more thermally and chemically time
stable than organic membranes and show both wide

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8 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13

soluble components. In what follows the main applications bovine serum, protein retention rates were 46%, 76%, and
of membrane processing in food processing are presented. 89%, respectively.
Yang et al. [79] have used low-cost ceramic MF mem-
4.1.1. Dairy processing industry branes elaborated from attapulgite, for the purification of
Ceramic membrane filtration in the food industry is cellulose fermentation fluid to improve the quality of
mainly applied in the dairy processing [68]. This process, cellulase products. They focused on the effect of the oper-
which is considered as the first membrane processing at an ating conditions and the membrane microstructure on the
industrial scale, appeared since the early 1960s [69]. Dairy decline in membrane flux. Results have shown that the
industry is based on applicability of membrane processes appropriate operating conditions were as follows:
driven by pressure (MF, UF, NF, and RO). As shown in Fig. 8, T ¼ 30 ± 3
C, DP ¼ 0.10 MPa, and flow velocity ¼ 4 m/s.
all major components of milk can be separated [70]. Raw Therefore, the attapulgite MF membrane having a mean
milk may be defined as polydisperse system with sus- pore size of 0.12 mm is appropriate for the treatment of
pended particles and soluble molecules, such as fat glob- cellulase fermentation fluid.
ules, casein micelles, whey proteins, lactose, and minerals.
These compounds may have different charges and sizes; 4.2. Beverages and drinking water
therefore, their separation by membrane processes can be
feasible [71]. Generally, MF with ceramic membranes is the The scope and frequency of beverage and drinking
most adopted technique for milk processing. It can be used water analyses are regulated in most countries. Besides,
for the concentration of milk and whey and also for the sensory testing and microbiological analysis compliant
elimination of bacteria [71]. Experiments have also been with limit values for impurities are most crucial. Among
conducted on milk protein concentration. Almandoz et al. these methods, we find the application of membrane pro-
[58] have fabricated tubular composite MF membranes cesses whose objective is to eliminate precipitates, micro-
from natural aluminosilicates (already cited previously) organisms, and suspended particles.
and tested for goat milk pasteurization. The obtained re-
sults show a high bacterial removal (87e99%). 4.2.1. Potable water
Likewise, Erdem et al. [72] have prepared a ceramic Water sustains human life and its purity cannot be
composite membrane based on alumina powder and tested compromised at any cost. However, conventional water
for whey protein separation. The obtained membrane has treatment processes including filtration, sedimentation,
shown good separation properties, with relatively high coagulation, and flocculation are not very effective in the
protein content and low lactose retention of about 80% and production of high-quality drinking water. Membrane
7%, respectively. filtration has been integrated in this area for meeting these
Also Popovi
c et al. [73] have investigated the perfor- stringent regulations. The production of drinking water by
mance of tubular ceramic membranes made of alumina the membrane process using a ceramic membrane has
during the filtration of whey reconstituted solution, been carried out since 1984 [80]. It is mostly used for
showing a PF reduction above 90%. removing precipitates, turbidity, suspended particles [81],
and then virus and bacteria from surface waters, such as
4.1.2. Protein separation and concentration rivers and lakes, when using a small-scale membrane
Protein concentration and separation is another sector treatment system [82e85].
for low-cost ceramic membrane application in food pro- The production of drinking water using ceramic filtra-
cessing, namely soymilk, fish, animal blood, egg, and gelatin tion membranes has recently attracted much interest. For
solutions [71,74,75]. Ishak et al. [76] have studied protein example, Alami-Younssi et al. [86] have shown that nitrate
separation and purification using hydrophilic modification ions can be removed from soft drinking water by NF
of alumina membranes. They changed the character of through an alumina membrane. Nevertheless, the poor
alumina (membrane active layer) from hydrophilic to penetrability of NF membrane has been a constraint for
superhydrophilic using graphene derivatives. The obtained industrial applications.
superhydrophilic ceramic membrane surface has a great MF using ceramic membranes was applied to reduce
impact on anticlogging and PF properties, and therefore it trihalomethane precursors from drinking water, remove
improves protein separation and purification process turbidity, and to act as disinfectant at the same time [6]. In
performances. the same vein, Ozdemir [87] has produced safe and quality
Kuca and Szaniawska [77] have investigated the per- potable water using the UF system through a porous
formance of separation processes by using a 150 kDa tubular ceramic membrane based on alumina. The treat-
ceramic membrane based on (Al2O3/TiO2 and ZrO2) for the ment of raw water has led to removing nearly 75% and 85%
recovery of proteins from the fish industry effluents. They of ferrous and turbidity contaminants, respectively.
showed that membrane process does not only reduce the Moreover, seawater desalination represents an increas-
biochemical oxygen demand and chemical oxygen demand ingly important solution to the rising drinking water scar-
(COD) from the fish industry salted wastewater but also city afflicting many of the world's regions. On the basis of
allows the recovery of high protein content (81%). this approach, ceramic membranes are often used because
Biron et al. [78] characterized tubular mullite ceramic of their high flux and stability. Zhu et al. [88] have investi-
membranes and then applied them in the separation of gated the desalination of seawater solution (0.3 wt% total
proteins. Depending on the filtration test of a protein so- dissolved solids) using zeolite membranes, which reached a
lution composed of trypsin and albumin from egg and high rejection (>93%) for all major seawater ions.

Please cite this article in press as: M. Issaoui, L. Limousy, Low-cost ceramic membranes: Synthesis, classifications, and appli-
cations, Comptes Rendus Chimie (2018), https://doi.org/10.1016/j.crci.2018.09.014
 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13 9

Fig. 8. Milk processing with membrane technology [70].

In another study, Gazagnes et al. [89] have desalinated characteristics was observed like color, clearness, and
sodium chloride solutions and seawater using a alcohol insoluble solid. The obtained clarified juice can
hydrophobic zirconia membrane (grafted with per- maintain its quality even for 30 days when refrigerated. Qin
fluorodecyltriethoxysilane). A high salt rejection rate et al. [94] have used three different low-cost fly ash pre-
(>95%) has been reached. cursor inorganic membranes for the clarification of centri-
fuged kiwi fruit juice. The evaluation of the permeation
4.2.2. Juice clarification and concentration characteristics proved that 1.25 mm was the optimal pore
Fruit juice clarification is one of the oldest separation diameter of membranes used in the clarification of kiwi fruit
processes using ceramic membranes [90]. This process can juice.
replace the conventional separation, thanks to its speed, Emani et al. [95] have synthesized low-cost inorganic
performance, labor reduction, as well the operation and MF membranes based on kaolin by the dry compaction
energy cost reduction. Comparing polymeric and ceramic method for the clarification of mosambi juice. Optimum
membranes in orange and lemon juice clarification, Capa- fabrication requirements have shown that the MF perfor-
nelli et al. [91] have concluded that ceramic membranes mance of the membrane fabricated at 49 MPa is highly
made from alumina as low-cost material could be more satisfactory for this application. A membrane flux of about
energy efficient than polymeric ones for industrial appli- 90 to 44  106 m3/(m2 s) at 206.7 kPa has been attained.
cations, giving higher PFs at a lower Reynolds number. The enzyme-treated centrifuged juice presents negligible
Nandi et al. [92,93] have studied the filtration of mosambi alcohol insoluble solid content.
and orange juices using a low-cost ceramic membrane based
on kaolin. They found that after MF test, essential properties 4.3. Alcoholic beverages
such as a total amount of soluble constituents of the juice,
pH, acidity, and juice density were almost unaffected. For many years, ceramic membranes have been used in
Although a significant improvement in other juice a large range beverage production. Experiments have

Please cite this article in press as: M. Issaoui, L. Limousy, Low-cost ceramic membranes: Synthesis, classifications, and appli-
cations, Comptes Rendus Chimie (2018), https://doi.org/10.1016/j.crci.2018.09.014
10 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13

shown that this can be extended to the clarification and advanced method for the treatment of oily wastewaters.
sterilization of alcoholic beverages. For instance, Youzhi Thus, the MF is a feasible and advantageous method for the
et al. [96] have filtered vinegar using low-cost tubular treatment of desalted wastewater effluent. According to the
ceramic membranes based on alumina. Optimization of obtained results, the ceramic membrane reaches high PF and
operation parameters shows that a membrane with a pore rejection, with the following experimental relationships: PF
size of 0.1 mm operating at room temperature under a increases with increasing volumetric flow rate, temperature,
transmembrane pressure of 0.14 MPa and a cross-flow ve- and pressure; however, it decreases with increasing oil
locity of 2 m/s is suitable for clarifying vinegar with high concentration. Rejection rises a little with increasing pres-
quality and low-haze potential even for 2 years. sure, salt concentration, and oil concentration, but it drops
with growing volumetric flow rate and temperature. The
4.4. Environmental applications results also show that the MF treatment is very effective in
the reduction of total organic carbon (TOC), total suspended
Over the past few years, extensive research was carried solids, and turbidity. Investigating the effects of different
out to develop low-cost ceramic membranes with high operating parameters leads to select the best operating
performance for different environmental applications, such conditions employing from 250 up to 3000 ppm of
as the treatment of dairy industry wastewater, oily wastes, condensate gas in water emulsions as synthetic feed. The
textile sludge, and other industrial wastewaters. In fact, the obtained reduction of TOC was greater than 94%.
use of ceramic membranes in the field of wastewater In another work, Abbasi et al. [102] have studied the
treatment is still limited because of their higher cost [97], effect of adding powdered activated carbon to mullite, on
as it is approximately 10 times higher than that of polymer the one hand, and mulliteealumina mixture (50/50 wt%)
membranes [98]. Hence, the need for a low-cost material on the other hand on TOC reduction. Their experimental
for the fabrication of ceramic membrane is needed. results prove that the addition of high concentration
Membrane process can be used for reducing the (1200 ppm) powdered activated carbon enhances the
amounts of wastewater polluting the environment and also elimination of TOC from 93.8% to 97.4 % and from 89.6% to
for the recovery of valuable substances from sewage. 92.4 % for mullite and mulliteealumina MF membranes,
Accordingly, new high quality porous ceramic membranes respectively.
elaborated from low-cost materials have been developed to Shokrkar et al. [103] have carried out experimental and
improve filtration efficiency, decrease energy usage, and modeling studies on the separation of oil from industrial
lower the amount of time lost on maintenance. Numerous oily wastewaters using mullite ceramic membranes man-
studies concerning wastewater treatments have been ufactured from kaolin clay and a-alumina powder. The use
elaborate. For example, Kumar et al. [99] have investigated of mullite ceramic membrane resulted in high TOC and COD
the treatment of wastewater generated by a local dairy elimination corresponding to 94% and 89%, respectively.
industry using a novel low-cost tubular ceramic mem- In another work, Nandi et al. [104] have treated oily
brane. They have manufactured a porous tubular ceramic wastewater using a low-cost ceramic membrane made
membrane via extrusion of natural clay paste, with 53% from inorganic precursors, such as kaolin, feldspar, quartz,
porosity, 0.309 mm pore size, and 5.93  107 m3/(m2 s kPa) boric acid, sodium carbonate, and sodium metasilicate. MF
of hydraulic permeability. Their results obtained from tests of synthetic oilewater emulsions with an initial oil
tangential MF process have shown that an increase in cross concentration of 250 mg/L show that the membrane can
flow rate and applied pressure lead to a decrease in the reach 98.8% oil rejection efficiency and 5.36  106 m3/
percentage of COD removal up to 91% (135 mg/L) in the (m2 s) PF after 1 h of filtration performed at 68.95 kPa
permeate stream with a flux of 2.59  106 m3/(m2 s), transmembrane pressure. Therefore, this ceramic mem-
which is well within the permissible limit for wastewater brane may be pertinent in the treatment of oilewater
discharge into the environment. These results prove the emulsions to yield permeate streams that can meet stricter
potential suitability of the fabricated ceramic membrane in environmental legislations (<10 mg/L).
dairy wastewater treatment to attain acceptable limit In the same vein, textile, paper, dyestuff, and laundry
(<200 mg/L) of the permeate stream. industries use large amounts of water and chemicals for
The main reason for wastewater treatments using a wet processing, and therefore generate several types of
ceramic membrane elaborated from low-cost materials has pollutants arising from the raw materials themselves and
been reported by Parma and Chowdhury [100]. They have also from the residual chemical reagents used for pro-
prepared circular disc-shaped membranes from locally cessing [105].
available clay (red mud with major constituents of silicon Because of the increasingly stringent restrictions on
dioxide (SiO2), aluminum oxide (Al2O3), and sodium oxide mineral and organic contents of industrial effluents, it is
(Na2O)) by paste casting method. MF tests have shown that necessary to eliminate the pollution load from wastewater
the resulting porous ceramic membranes are convenient before it is discharged to the environment. Several works
for oily wastewater treatment. The ones sintered at 800
C have been conducted for the treatment of colored waste-
have reached a maximum rejection rate of 53% for crude oil water using a low-cost ceramic membrane. For instance,
from crude oilewater emulsion. Jedidi et al. [22] have elaborated tubular ceramic mem-
Abbasi et al. [101] have synthesized ceramic membranes branes based on coal fly ash mineral. The obtained filters
from kaolin clay and studied their performances in MF. It was were used in the treatment of dyes present in wastewater
shown that mullite ceramic membrane manufactured by resulting from the wash baths of the textile industry. Table 2
extruding and calcining kaolin clay can be used as an presents the results of MF using the elaborated ceramic

Please cite this article in press as: M. Issaoui, L. Limousy, Low-cost ceramic membranes: Synthesis, classifications, and appli-
cations, Comptes Rendus Chimie (2018), https://doi.org/10.1016/j.crci.2018.09.014
 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13 11

membrane compared with a commercial alumina mem-

brane. It has been found that MF results using a fly ash
membrane proved to be effective as that obtained with an
alumina membrane in removing the COD, turbidity, and
color from wastewater. The conductivity as well as the
turbidity and the absorbance of the solution were a little
less than the one obtained with the commercial membrane,
whereas the COD concentration was a little bit higher. This
can be explained by the selectivity of the fly ash membrane,
which can be different from the commercial one because of
specific surface properties, like electrostatic interactions
that can be different than the properties of the commercial
membrane because of their chemical composition.
Issaoui et al. [19] have prepared porous flat cermet
membranes from kaolin and aluminum powders. The
membranes were then tested for the filtration of an indigo
Fig. 9. Results of decolorization obtained after the filtration of an aqueous
blue solution. The dead-end filtration results show that it is
solution containing the Indigo blue dye (T ¼ 25
C, P ¼ 6 bar): permeate
possible to completely remove the color of the initial so- solution (on the right), retentate (in the middle), and the initial solution (on
lution (containing blue dye), with a significant retention of the left) [19].
dyes in the concentrate and a complete discoloration of the
solution (Fig. 9). For their part, Hasan et al. [109] have developed a low-
Silva et al. [106] have used inexpensive raw materials, cost membrane bioreactor (MBR) made of 80% clay soil and
namely, kaolin and ball clay to synthesize tubular ceramic 20% rice bran. They showed that the obtained hollow cy-
membranes and used them in the treatment of textile in- lindrical ceramic filters would be appropriated for waste-
dustry wastewater. Their results show the effectiveness of water treatment, removing arsenic from groundwater.
the elaborated ceramic membranes with a decrease in Further research in the field of environmental protec-
turbidity and discoloration, reaching approximately 100% tion using membranes has been conducted, for example,
of rejection of the solid particles. Zorpas [110] investigated the combination of MBR and
In the same context, Nasir and Faizal [107] have inves- chemical oxidation process for the treatment of household
tigated an alternative treatment for removing cadmium heating wastewater. The results prove that the immersed
from pulp industry effluent using ceramic membranes hollow fiber module (with a nominal pore size of 0.04 mm, a
elaborated from a mixture of 87.5% natural clay, 10% rice total membrane surface area of 0.047 m2, and made from
bran, and 2.5% iron powder. The results show that these polyvinylidene difluoride) combined with a reactor was
membranes were able to reduce cadmium concentration found to be a more promising process than the application
up to 99%. of Fenton oxidation technique for the effluent discharge
In another study, Han et al. [108] have prepared ceramic with the least environmental impact.
membranes from dewatered sludge, fly ash, and clay. Water In the same vein, Aileen and Albert [111] have studied
filtration tests showed that heavy metals were not leached modeling MBR systems, specifically for municipal waste-
during the filtration process, which proved that the ob- water treatment, which can yield high-quality water with
tained ceramic filters were safe for wastewater treatment. reported removal percentages of 95%, 98%, and >99% for
This was associated with the solidification of heavy metals COD, biochemical oxygen demand, and total suspended
in the form of metallic oxides during the calcination process. solid, respectively.
Other low-cost tubular composite ceramic membranes have Also, Zhang et al. [112] have used a flat stainless steel
been fabricated by Almandoz et al. [58] using natural alu- membrane with homogeneous and tighter pore size in an
minosilicates (previously mentioned). Their investigations experimental submerged MBR for the treatment of syn-
have shown that composite tubular membranes were thetic domestic sewage. The used membrane was quite
suitable for wastewater treatment. The obtained results effective in the elimination of organic substances and COD
have shown an insoluble residue rejection of 100% and high removal efficiency achieving 97%. Thus, the use of stainless
bacterial removal ranging from 87% to 99% of slaughter- steel membrane in a MBR for wastewater treatment is
house wastewater treatment and goat milk pasteurization. economical.

Table 2 5. Ceramic membrane cost

Results of the effluent before and after MF at 1 bar: using ash and com-
mercial alumina membranes [22].
Industrially, the competitive aspect of membrane tech-
Sample Conductivity Turbidity COD Absorbance nology lies in its cost. Indeed, some conventional ceramic
(ms/cm) (NTU) (mg/L) at 600 nm membranes available for industrial scale operation are
Raw effluent 6.16 45.5 3440 0.104 expensive, including manufacturing and raw material costs.
Fly ash membrane 5.38 0.58 880 0.010 An a-alumina porous tubular ceramic membrane with
permeate average pore diameters varying from 1000 to 6000 nm costs
Alumina membrane 5.6 0.62 834 0.013
between $500 and $1000/m2 (Ce
ramiques Techniques,
permeate
2007).

Please cite this article in press as: M. Issaoui, L. Limousy, Low-cost ceramic membranes: Synthesis, classifications, and appli-
cations, Comptes Rendus Chimie (2018), https://doi.org/10.1016/j.crci.2018.09.014
12 M. Issaoui, L. Limousy / C. R. Chimie xxx (2018) 1e13

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Please cite this article in press as: M. Issaoui, L. Limousy, Low-cost ceramic membranes: Synthesis, classifications, and appli-
cations, Comptes Rendus Chimie (2018), https://doi.org/10.1016/j.crci.2018.09.014