Journal of Industrial and Engineering Chemistry 109 (2022) 100–124

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Journal of Industrial and Engineering Chemistry

journal homepage: www.elsevier.com/locate/jiec

Review

Novel polymeric additives in the preparation and modification of

polymeric membranes: A comprehensive review
Nazanin Nasrollahi a, Leila Ghalamchi a, Vahid Vatanpour b,c,⇑, Alireza Khataee d,e,⇑, Maryam Yousefpoor f
a
Department of Applied Chemistry, Faculty of Chemistry, University of Tabriz, 5166616471 Tabriz, Iran
b
Department of Applied Chemistry, Faculty of Chemistry, Kharazmi University, 15719-14911 Tehran, Iran
c
Environmental Engineering Department, Istanbul Technical University, Maslak, Istanbul 34469, Turkey
d
Research Laboratory of Advanced Water and Wastewater Treatment Processes, Department of Applied Chemistry, Faculty of Chemistry, University of Tabriz, 51666-16471
Tabriz, Iran
e
Peoples’ Friendship University of Russia (RUDN University), 6 Miklukho-Maklaya Street, Moscow, 117198, Russian Federation
f
Department of Mineral Chemistry, Faculty of Chemistry, Iran University of Science and Technology, Tehran, Iran

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

Article history: One of the basic challenges in polymeric membrane fabrication is the control of pore size and the porosity
Received 27 November 2021 of the membranes. In this review paper, the role of polymeric additives is overviewed in membrane fab-
Revised 16 January 2022 rication processes, such as the formation of pores in membranes, increasing permeability, hydrophilicity
Accepted 16 February 2022
and even the creation of a desirable property such as antifouling and antibacterial properties. The poly-
Available online 24 February 2022
meric additives could dissolve in water during the phase inversion process (a pore forming agent) or
remain in the membrane matrix (hydrophilic and antifouling agent) or could have both roles. The addi-
Keywords:
tives could also act as proton exchanger and gas transport facilitating agents. This review concentrates on
Membranes
Additives
the introduction of new polymeric additives. In the blended membranes, the miscibility of chosen poly-
Miscibility meric additives at the molecular levels make it a challenge to use the modification method. Molecular
Phase inversion interactions between polymers such as hydrogen bonding and charge transfer play the main roles of
Pore former the quality of blending. Different methods of polymer/co-polymer addition to the polymeric matrix of
membranes are investigated to identify the best polymeric additives in various types of polymeric mem-
branes including: pervaporation, contactor membrane, distillation membrane, etc. Moreover, the mixa-
bility of the additive polymer with the matrix polymer solution and the effectiveness of some
functional additives are described in this review.
Ó 2022 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights
reserved.

Contents

Introduction. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 101
Polymer blending/composite . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 102
The role of additive polymers. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 103
Hydrophilic agents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 104
Pore former . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 105
Water-soluble polymeric (WSP) pore formers. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 105
Applications of pore formers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 107
Proton exchangers. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 108
Gas solubility agents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 111
The role of polymeric additives in gas separation membranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 111
PEG additive . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 112
Polyurethane additive . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 112
Polyimide (PI) additive . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 113

⇑ Corresponding authors.
E-mail addresses: vahidvatanpour@khu.ac.ir (V. Vatanpour), a_khataee@tabrizu.ac.ir (A. Khataee).

https://doi.org/10.1016/j.jiec.2022.02.036
1226-086X/Ó 2022 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al. Journal of Industrial and Engineering Chemistry 109 (2022) 100–124

The role of polymeric additives in liquid filtration membranes. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 113

Phase inversion membranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 113
Interfacial polymerization (IP) membranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 116
The role of polymeric additives in ion-exchange membranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 117
The role of polymeric additives in distillation membranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 118
The role of polymeric additives in pervaporation membranes. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 118
The role of polymeric additives in contactor membranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 120
Polymeric nanoparticle additives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 120
Conclusion and perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 120
CRediT author statement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 120
Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 120
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 121
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 121

Introduction able membrane in the kind of reverse osmosis, pervaporation,

A membrane is described as a thin layer that has mass transport
in a selective manner. Numerous varieties of organic and inorganic
materials have been used to fabricate the membranes. The revolu-
tion in the industrial usage of membranes resulted from mem-
brane materials and structures, as well as the production of
membranes in the large scale. For the use of membranes in an
industrial scale, they should have the following properties at the
lowest [1]: high permeability, high selectivity and rejection, good
mechanical strength, high stability at high temperatures, low fab-
rication cost, and the ability to package and module fabrication
in a high surface area. However, only a few polymers such as
polyvinylidene fluoride (PVDF) [2], polysulfone (PSf) [3], polyether-
sulfone (PES) [4], polyvinyl chloride (PVC) [5] and cellulose acetate
(CA) [6] have some of these properties. To reach or improve other
characteristics, the polymeric or inorganic additives are usually
blended in the matrix of the main polymers.
Fig. 1 shows a classification scheme based on some properties
such as their geometry, bulk structure, production method, sep-
aration regime, and applications of synthetic membranes. Gener-
ally, porous membranes are used in different applications of
membranes. High porosity and limited size distribution of pores
in porous membranes make them the prominent choices. A suit-
and the gas separation process must have a dense and selective
layer for proper application. The solution/diffusion is the applied
mechanism for the permeation of dense membranes [7]. More-
over, the stability of long-term separation properties such as
permeability, selectivity, and rejection, are the main characteris-
tics of selection.
Symmetric (isotropic) and asymmetric (anisotropic) structures
are different kinds of polymeric membrane structures. Throughout
the whole membrane thickness, the symmetric membrane has a
uniform structure. Whereas, gradation in the structure of mem-
branes was observed in asymmetric types. Furthermore, the dense
region in the polymeric membrane was primarily used to specify
the separation property of membranes in the asymmetric type.
With the control of phase inversion conditions, it is possible to pre-
pare polymeric membranes with both symmetric and asymmetric
structures. The addition of polymeric additives to the casting solu-
tions of membranes could influence the exchange rate between the
solvent and non-solvent during the coagulation process and could
increase or decrease the porosity, hydrophilicity, pore size, and
morphology based on the additive properties and concentrations
[8–10]. In recent years, the number of articles on polymer blending
membranes has grown rapidly. The increasing attention to this
field, shows that the physically blending of two or more polymeric

Fig. 1. The categorization scheme of fabricated membranes based on their main properties: geometry, bulk structure, production method, the structure of the separation
layer and application.

101
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
Fig. 2. Schematic representation of polymer blends [13].
materials results in new composite materials with improved
properties.
This study, comprehensively reviews the use of polymeric addi-
tives in the fabrication of different polymeric membranes applied
for both liquid and gas filtrations. There are some review papers
about the use of additives in membrane fabrications [11–14] How-
ever, they are usually focused on the fabrication of membranes for
a special application such as gas separation [11], and pervaporation
[13] or concentrate on a famous pore former including PEG [11]
and PVP [14]. This review, highlights the application of newly syn-
thesized polymeric additives in the fabrication of membranes
reported in recent and past years [15–17].
Polymer blending/composite
In recent decades, several kinds of polymer materials have been
used to develop membrane technology [13,18] (Fig. 2). Aiming at
overcoming the deficiencies of polymers in individual forms. To
know more details about Fig. 2, the fractional free volume (FFV)
is explained for the total fraction of unoccupied space in the poly-
meric based materials and its usage in blending membranes. The
FVV includes more or less solitary spaces of different sizes and vol-
umes. The free volume in polymeric system can be modified by the
addition of additives (such as pore formers) to the polymeric
matrix of a membrane, and consequently, changes will occur in
the permeability and selectivity.
Generally, the following equation is used to calculate FFV:
V  V0
FFV ¼
V
where V (cm3/g) is defined as total molar volume of the repeating
unit, which is calculated from density (1/q). V0 is the volume occu-
pied by polymer chains (cm3/g) and obtained from:
Xk
V 0 ¼ 1:3 k¼1 ðV w Þk
where K is the summation of group numbers in repeating unit, (VW)k
is the volume of van der Waals in the structure of various polymer
Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
groups. The van der Waals of blending polymers (Vwb) were also cal-
culated by the following equation:
V wb ¼ w1 V 1 þ w2 V 2 ð3Þ
where w1, w2, V1 and V2 relate to the weight fractions and van der
Waals volumes of ingredient 1 and 2, respectively. For the polymer
blends, the FFV was determined by a mixing manner:
FFV b ¼ w1 FFV 1 þ w2 FFV 2 ð4Þ
where FFV1, FFV2 and FFVb are the FVV of incorporated components
1, 2 and the blending polymer respectively.
Furthermore, the new composition has been widely investi-
gated to develop membranes with pleasing morphology and chem-
istry for better performance in separation and module designs [19–
21]. For better development with minimum risk, fabrication cost
and duration, one of the most feasible strategies can be the modi-
fication of membrane materials. Especially about membranes for
gas separation, high permeability has always a direct relationship
with low selectivity making them limited for use on industrial
scale [21]. In recent decades, several strategies such as cross-
linking, polymer blending, and using mixed matrix membranes
have been used to overcome this problem [13,20–22].
It has been well known that the morphology can be controlled
by adding small amounts of additives. Polymeric additives are
widely added in low concentrations within the main polymeric
matrix for the structure control of membranes. The dispersed
phase (polymeric additive) is identified by its fewer amounts to
the main polymer of a membrane and should also be precisely
ð1Þ determined by various shapes and sizes and their compatibility
with the main polymer phase. The typical criteria involved are:
(a) additive dispersibility/solubility in the continuous matrix; (b)
compatibility of the additive with the main polymer matrix and
(c) physical and surface properties of both phases.
Polymer blending is discussed to be one of the most famous
ð2Þ methods. In addition to a new positive property derived from a
combination of selective polymers, an undesirable property
defined as the miscibility of blending at the molecular level about
combining polymers can be omitted in this technique [23]. On the
102
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
Fig. 3. Schematic to present classification in polymer blends: miscible, partially miscible and immiscible [13].
other hand, the miscibility of the chosen polymers at the molecular
levels makes it a challenge to use the noted technique. On the
whole case of dispersion, the morphology of different polymers,
phase adhesion, and consequently the obtained properties of final
mixtures depends on the thermodynamics of different polymers
[24]. The miscibility of polymers can be classified into three differ-
ent categories: miscible, immiscible and fractionally miscible
(Fig. 3). In a homogenous system, two materials are blended at
the molecular level and create one phase due to the hydrogen
bonding or physical interactions. In an immiscible blending sys-
tem, the interface between two or more components and the
impossibility of solving are their distinctive features. In a partially
blending system, the partially dissolving of components in each
other makes a heterogeneous phase. Furthermore, when the com-
position of involved components is dissimilar to the primary fea-
tures of components, it is called an isotropic heterogeneous
system. Between different blending phases, a miscible blend
results in a uniform and stable performance, as well as, thermal
and mechanical features of products. Choosing a second polymer
is one of the key factors in polymer blending system to obtain
favorable physical and chemical properties.
Commonly, dispersion in the molecular scale, phase adhesion,
the morphologicy property of two-phase integration and conse-
quently, the final properties of products depend on the thermody-
namics of polymer blending. Polymer blending based on
miscibility can be classified into three groups defined as miscible,
immiscible, and fractionally miscible [23].
Stable thermal and mechanical properties and the improved
performance of blended membranes are the conclusions of a mis-
cible blend system. One of the effective strategies in polymer
blending is the choice of the right source with favorable chemical
and physical properties. ISI web of science, shows that the number
of published papers with polymer blend membranes is increasing,
rapidly. Paul and Newman published one of the best review articles
on polymer blends in 1978 [25]. Moreover, Lloyd M. Robeson pub-
lished an excellent review about polymer blends. They discussed
comprehensively thermodynamics, phase behavior and the modifi-
103
Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
cation of the chosen polymer to blend as well as their new proper-
ties and applications [26].
The miscibility of polymer blends is related to the molecular
interaction between the chosen polymers such as hydrogen bond-
ing and charge transfer interactions. Fig. 3 shows the brief sche-
matic of this miscibility. Fourier transform infrared spectroscopy
(FTIR) is usually used to investigate about hydrogen bonding
between two polymers. After blending, applying FTIR also helps
to indicate the happened interactions. Another possible interaction
between two polymers is charge transfer complexes (CTCs), in
which two essential parts are electron-pair donor and acceptor
[27]. This phenomenon is not limited to polymer blends and is
widely used in other applications such as optical tensile, semi,
super and electrical conductors and solar cells. It is generally
known that aromatic polyimides are one of the interactive group
of compounds to form intermolecular and intramolecular CTCs.
The power of CTCs is generally examined using an absorption band
fluorescence spectrophotometer and UV spectroscopy generally
applied. After polymer blending, a new distinct adsorption band
usually illustrates the formation of intermolecular CTCs. Some-
times, hydrogen bonding between polymeric molecules, reacts as
a cross-linking structure and changes the glass transition temper-
ature (Tg) to a more value. Furthermore, it is claimed that an
increase in the Tg of polyimides can be due to the formation inter-
chain CTCs during the crigidifying of a polymer [28].
In the following parts, a comprehensive review is presented
about different kinds of polymeric additives and their effective
roles in various membrane technologies.
The role of additive polymers
Diversity, simple preparation methods, and ease to scale-up are
the main properties of polymers to change them as attractive
materials for membrane technology. Nowadays, numerous types
of polymer materials are used to develop membranes. In addition
to applying new membrane materials [29,30], the desirable chem-
istry and morphology as well as separation performance in differ-
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
ent scales from laboratory to module designs, have attracted atten-
tion for many researchers [31]. To make an equilibrium between
improving separation performance, risk, cost, and duration; chang-
ing membrane materials seems to be a more practical strategy.
Among different modification methods of membrane materials,
such as blending of polymers, mixed matrix membranes (MMMs),
and cross-linking, polymer blending attracted more attention
because of its special property to combine individual properties
of different polymers to obtain a new composite with targeted per-
formance and overcome undesirable properties of polymers in the
separated mood [12]. It should be mentioned that the thermody-
namics of polymeric additives are the main factor in the dispersion
of molecular state, the morphology of two polymer phases in the
mixture, and phase adhesion, eventually influencing the final prod-
ucts [32,33].
Hydrophilic agents
In the fabrication of blended membranes, the presence of addi-
tives in a polymer stock solution is an attractive method in the
membrane industry to increase hydrophilicity to improve mem-
brane performance such as permeability, rejection, and reduction
of fouling [34]. Two main categories exist for embedding additives
including (i) polymers and (ii) inorganic nanoparticles (NPs)
[35,36]. Suggested polymers including polyvinylpyrrolidone (PVP)
[37], polyethylene glycol (PEG) [38], chitosan (CS) [39], polyamide
(PA) [40], polyethylene oxide (PEO) [41], etc. There are some
papers that introduce novel polymeric additives with huge struc-
tures [40,42] and dendrimer chemistry [43,44] to trap in the main
polymer body and increase membrane hydrophilicity and antifoul-
ing properties. Jalali et al. [42] introduced a novel additive i.e. a
polysulfide-amide (PSA) copolymer (Fig. 4a) to increase the
hydrophilicity and performance of the resulting microporous PES
Fig. 4. (a) The huge structure hydrophilic agent of polysulfide-amide (PSA) copolymer addition in PES membrane structure [42], (b) aromatic carboxylated polyamide [45], (c)
thiazole based aromatic polyamide with big naphthalene groups [40].
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
membranes. The presence of nitro groups, thiazole rings, and
thioether linkage increased the hydrophilicity and porosity of the
obtained PES membranes. Rezania et al. [45] synthesized car-
boxylic acid containing polyamide (CPA) (Fig. 4b) and blended it
into a PES/DMAc casting solution. The CPA presence in the matrix
of the membrane augmented water flux while it reduced protein
fouling. They also measured the membrane contact angles to eval-
uate the differences in the hydrophilicity of the bare and blend
membranes. According to their results, the bare PES membrane
showed the utmost contact angle (73.4°), while, a decreasing trend
was gradually observed for the water contact angle by the CPA
addition in higher concentrations. The decreasing trend was attrib-
uted to the hydrophilic tendency of carboxylic acid groups in the
CPA structure that established hydrogen bonds with water mole-
cules and reached to 60.9° as the minimum water contact angle
for the blend membrane. This result confirmed that CPA could be
considered an effectual agent to improve the hydrophilicity of
PES membranes.
The resulting PES/CPA membrane exhibited more porosity,
hydrophilicity, and higher vertically finger-like pores than the
unfilled PES membrane. Shockravi et al. [40] prepared an asym-
metric PES UF membrane using an aromatic polyamide with large
additive of naphthalene groups (Fig. 4c). Higher permeability,
porosity and antifouling properties were obtained with co-using
of the aromatic polyamide and PVP. These bulky additives could
trap in the host polymer chains and remain in the membrane
structure, thereby improving the membrane hydrophilicity and
antifouling properties.
Other methods of increasing the hydrophilicity of membranes
include in situ polymerization and in situ cross-linking methods
for maintaining hydrophilic agents on the host polymers [46].
Zhu et al. [47] fabricated a PVDF membrane via cross-linking poly-
merization to increase the hydrophilicity of membranes for
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al. Journal of Industrial and Engineering Chemistry 109 (2022) 100–124

Table 1
Progress of recent studies for fabrication of hydrophilic polymer blend membranes.

Polymer Additive Additive Contact angle Performance change by bending the additives Reference
base loading (%) change (°)
PES PA-6 + PVP 2 76 to 68 – PA-6 exhibited good compatibility with the PES [40]
– By increasing PA-6 content, hydrophilicity, permeability and antifoul-
ing enhanced
PES PVP 2 76 to 71 Pure water flux of PVP added membranes were higher than bare one. [42]
PES PEG/PVP 2 85 to 59 – Morphology drastically changed from finger-like to homogeneous [50]
sponge-like
– Enhancing hydrophilicity and permeability
PES PVP 40 K 2–10 71 to 47 – Enhanced permeability for membranes prepared with lower PES [51]
concentration
– For the higher PES concentration, after a specific PVP loading, the per-
meability reduced due to obtaining denser structure
PES Pluronic 31R1 5 63 to 44 Enhancing permeability, and antifouling properties [52]
PVP 5 63 to 56
PES N-phthaloyl-chitosan 0.9 61 to 56 – Improved permeance and hydrophilicity [53]
– Improved BSA solution flux
– But relative flux loss and recovery were not significantly changed.
PES Aliphatic dithiocarbamate 0.5–5 61.2 to 48.4 – Improved permeance and hydrophilicity [54]
Aromatic dithiocarbamate 0.5–5 61.2 to 47.8 – Improved antifouling properties
– Improved arsenic removal
PVDF Amphiphilic PVDF-b-PEG-b- 2–5 105 to 39 – Additive acts both as a surface modifying and pore forming agent [55]
PVDF – Improved permeance and hydrophilicity
PSf Polyethylene glycol methyl ether 1–9 64 to 46 Improved hydrophilicity, permeability and antifouling property [56]
(PEGME), MW = 5000
PSf Styrene-maleic anhydride 1 86 to 69 Improved hydrophilicity, permeability and antifouling property [57]
copolymer + PEG

increasing the separation efficiency of water-in oil. Polymer-
polymer blending was performed in membrane preparation
technology to modify the performance of membranes due to an
enhanced flux. The preparation of super-hydrophilic zwitterionic
PVDF with poly(3-(n-2-methacryloxethl-N,N-dimethyl)
ammonatopropanesultone)-co-2-hydroxyethylmethacrylate was
also reported via the fabrication of membranes by NIPS method
[48].
In the polymer addition method, two or more types of polymers
are blended into the dope solution to change the polymer contents
and induce the wettability, functionality of the membrane surface
and the resulting hydrophilicity. Masuelli [49] studied the pres-
ence of polycarbonate (PC) in PVDF solutions to increase mem-
brane performance. A slight alteration in mean pore size was
reported with enlarging the PC amount, nevertheless a consider-
able change was reported the surface structure and porosity of
membranes. Table 1 summarizes some examples of fabricating
hydrophilic polymer blend membranes.
Pore former
In general, gravimetric porosity, pore size and pore size distri-
bution are a group of the most important morphological parame-
ters. Gravimetric porosity is a kind of measurement to calculate
the total amount of void in a membrane. It presents the ratio
between the membrane density and the density of the neat matrix
[58]. Pore size represents the dimensions of the pores, which are
the channels of a variable cross-section. The distance between
two opposite pore walls is known as the pore size for simple geo-
metrics. If the pores have irregular shapes, some averaging is made
to report an average pore size. In general, an equivalent spherical
shape is assumed, but other proposed representations include
cage-like/spherical mesoporous structures, non-spherical particles,
etc. [59,60]. Since the pores do not all have the same size and/or
geometry, some statistical analyses must be performed using a
105
model such as nonlinear optimization and Monte Carlo integration,
to obtain a representation of pore size distribution [60].
In recent decades, fabricating polymeric membranes with the
especial property of being a porous or dense framework has
attracted significant attention. To have a brief definition, the ratio
of pore volume to the total volume of a porous membrane is poros-
ity which is evaluated as a significant parameter. Lower resistance
to the solvent flow is the result of more porosity of the sub-layer
through the membrane. More amounts of pore numbers or an
increase in their average diameters, are eventuated in higher sur-
face porosity. It should be mentioned that, porosity is an important
feature of membranes due to selective filtration, so that it
improves the performance of porous membranes deserve special
attention.
Up to now, various methods such as: 1) adding a pore former
during the polymerization, 2) using thermally unstable compo-
nents in a polymer blend, and 3) using selective decomposition
of thermally unstable block copolymers were applied [61]. PVP
and PEG are the two water-soluble polymers that are greatly used
as additives through the fabrication of polymeric membranes via
the phase inversion method because of their high compatibility
with water and organic solvents as well as small toxicity. These
polymers, are usually water-soluble, and this special property
results in increasing the membrane pore surface and the pore-
forming effect.
Water-soluble polymeric (WSP) pore formers
The water solubility of synthetic WSPs is due to their hydrophi-
lic groups to increase the stability and strength of the casting solu-
tion. The most common synthetic WSPs are PVP, PEG, and PVA
[62]. Actually, the fabrication of a ‘‘hydrophilized” membrane is
approached by the addition of PVP and PEG for the fabrication of
a casting solution to access the customary approach. It should be
mentioned that using organic acids, such as propionic acid and
acetic acid usually form macrovoids.
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
Zheng et al. [63] used PEG as an additive in a PSf solution and
studied the kinetics of membrane formation, and variations in rhe-
ological and thermodynamic parameters of membranes. Based on
their published results, PEG addition changed the thermodynamic
instability and rheological barrier properties of the PSf casting
solution in a positive trend. In a similar study, Boom et al. [64] used
the PVP polymer additive in the PES polymeric matrix and NMP as
a solvent. They declared that adding PVP, reduced the possibility of
delayed demixing and the formation of macrovoids. Different types
of PVP were used mainly to produce highly porous membranes
[65] such as cross-linked PVP, copolymers and homopolymers
(with different molecular weights). Li et al. [66] used PVP as an
additive for a PVDF hollow fiber membrane and observed a signif-
icant growth in the porosity of fabricated membranes. However,
using PVP as the additive, didn’t change the mean pore size of
the membrane. In a similar study, Fontananova et al. [67] studied
the effect of PVP addition to the PVDF polymeric matrix and
observed a similar modification. The same results were obtained
in PVDF hollow fiber membranes and PVP addition by Mansour-
izadeh and Ismail [68]. Rhee et al. [69] used various molecular
weights of PVP in the casting solution of hollow fibers of polyether-
imide (PEI), and concluded that the addition of PVP in a higher
molecular weight resulted in pores with a larger size. In a similar
study, Hilal et al. [70] decreased the PVP concentration and
reported lower water flux and higher rejection. It should be noted
that PVP addition to the PES membrane, made higher water flux
but decreased the water contact angle [71]. Rahimpour and
Madaeni [72] reported a significant increase in membrane perme-
ability by PVP addition to a PES UF membrane with no changes in
selectivity. The addition of PVP resulted in more pore density of
membranes and decreased the membrane dense layer and effec-
tive thickness because of forming macrovoid in the support layer.
Moreover, an increase in the membrane surface and hydrophilicity
of pores are the other advantages of PVP addition. Many scientists
discussed more details of the formation of macrovoids, which are
elongated spaces and present under the upper surface of the mem-
brane [73]. For the PSf membrane, blending with hydrophilic addi-
tives in the casting solution resulted in better performance along
with higher permeability and antifouling property [74]. Further-
more, PVP is used in drug delivery and ultrafiltration (UF) applica-
tions and usually in medical and food industries with no reported
toxicity reported [75].
PEg. One of the prominent polymeric additives is PEG. Low nature
toxicity and solubility in water are the two main properties of PEG
making it an important material in biological applications. More
porosity is the result of PEG addition to the PSf membrane [74].
A special growth in pure water flux with low rejection was
obtained by the addition of PEG as the pore former to the mem-
brane matrix. This effect could be reversed by heating for more
than 10 min [71]. Arthanareeswaran et al. [76] used low molecular
weight PEG as an additive in a polymeric solution, and observed an
enhancement in porosity/permeability by increasing PEG contents.
Saljoughi et al. [77] changed the concentration of PEG between 0
and 10 wt% and a temperature from 0 to 25 °C. They reported that
pure water flux and BSA rejection increased due to increasing the
PEG concentration, along with more macrovoid formation in the
sublayer of the membrane. Chen et al. [78] confirmed that the addi-
tive concentration was one of the most impressible parameters
that should be paid special attention to have better membrane per-
formance. They also studied the performance of a PEI polymeric
membrane using PEG as an additive. PEG addition with different
contents altered the morphological structure of membranes. More
concentration of the additive elevated the average pore radius of
the PEI membrane. Moreover, pore distribution and the number
of pores increased with vanishing the macrovoids [79].
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
In another study, Fan et al. [80] reported that PEG addition at
low concentrations to a PVC membrane, resulted in a finger-like
structure formation, whereas a higher concentration created a
spongy structure in the membrane. The fabricated membrane pos-
sessed higher permeability, and better stability in chemical and
mechanical properties for the UF application.
Polyvinyl alcohol (PVA). 1,3-Diglycol polymer or PVA has numerous
applications because of a simple preparation method, easy film-
making, thermal stability, mechanical strength, flexibility and the
best hydrophilicity. The biodegradable property of PVA makes it
a suitable component in the paper and textile industry [81]. Blend-
ing with PVA enhances the mechanical property and hydrophilicity
of bio and other polymers [82]. In addition, PVA is applied as a pore
former in sol–gel bio-glasses. The produced pores by the cited
method are larger than 100 lm [83]. Rambo et al. [84] investigated
the increase of alumina porosity to 86% due to PVA addition. Their
BET surface area was calculated as 3.6 m2.g1. Liu et al. [85] fabri-
cated a polymer with an adsorptive property (the same as chi-
tosan) modified by PVA, cellulose acrylonitrile butadiene acetate
and styrene for heavy water removal. An enhancement in the pore
size of ethyl cellulose film-coated pellets by the addition of PVA to
the bulk material resulted in the increase of the hydrophobic drug
dipyridamole release from the pellets [86]. PVA improved the per-
formance of chitosan/PVA/zeolitic imidazolate framework (ZIF-8)
thin membrane adsorbents for dye removal [87]. Furthermore,
PVA addition improved CO2 separation from water more efficiently
[88].
Polyacrylic acid (PAA). PAA is biodegradable synthetic WSP poly-
mer. That is also used as an adsorbent for purification in water
treatment. It has a unique behavior among pore formers because
of its liquid phase at pH 5 and changes to the gel phase at pH 7
[89]. Different researchers investigated the effect of adding PAA
to the polymeric matrix of membranes. Li et al. [89] used PAA as
a pore former in a PI membrane and reported the enhancement
of porosity. M’Bareck et al. [90] fabricated PAA/PSf membrane
and reported a pure water flux of 18 L.m2.h1 and Ponceau S
dye rejection rates of about 90% and 99%, respectively. Further-
more, He et al. [91] synthesized a PAA/PC composite membrane
and used it for surface modification of a tubular-type reactor. de
Oliveira et al. [92] fabricated a polymeric membrane in a compos-
ite type by mixing PAA and CS as a cation in various contents. They
reported the use of more contents of PAA in a blend.
Polyacrylamide (PAM). PAM is a synthetic type polymer synthe-
sized by the polymerization of a monomer acrylamide is named
neurotoxin. Its unique property is stability in a broad range of
pHs (from 3 to 11). The application of PAM is very different includ-
ing: drug delivery (soft-coated gelatin capsules, stable delivery of
insulin, and transdermal penetration of injective drugs to skin),
cosmetic products, macro-fractionation, and microanalysis of
nucleic acids, and electrophoretic proteins. The combination of
PAM hydrogel with hydrogel is a biocompatible compound and
used for sustained antibiotic release [93,94].
Zhang et al. [95] used a PAM membrane caused by the polymer-
flooding process for wastewater treatment. To remove oil from the
reservoir, polymer flooding is known as a prominent method. PAM
is one of the most common components used as an agent for
polymer-flooding. However, it should be mentioned that when
PAM is used as an agent in polymer-flooding, a significant amount
of PAM is considered in permeated water. More contents of PAM
affected the pore size of membranes and, consequently, changed
their pure flux. A NaOH solution (pH > 12) was also used to study
the fouling mechanism of PAM membranes. In the case of waste
water treatment, the dispersion of oil and solid in hydrolyzed
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
PAM residue, made a problem and affected its performance. Wang
et al. [96] studied the case of conclusive flux and the effect of main
pollutants on polymer-flooding wastewater in an oil-filled manner.
The smaller size of PSM, which decreased of membrane efficiency,
was due to a high concentration of salt. It is explained by repulsion
in the PAM molecules, which was screened by more presence of
ions in highly concentrated salt solution [97]. El-Reash et al. [98]
synthesized a CS-PAM membrane and studied the thermal stability
growth of CS by enhancing PAM contents in it. Furthermore, they
reported that the fabricated membrane could be used for the
removal of adsorptive Cu(II). Moreover, they reported that adding
PAM to its matrix increased the antimicrobial activity. Nasser
et al. [99] reported a slight reduction in the hydrophobicity of poly-
ether ether ketone (PEEK) by adding PAM. Akbari et al. [100] used
TiO2 as a filler in the matrix of PAM membranes and reported pure
water flux growth of about 31.2% and better antifouling property
due to more hydrophilicity of blended membranes. Zhang et al.
[101] fabricated PAM-polydivinylbenzene membranes and
observed improved pH stability, separation efficiency (about 90%)
and scaling up.
N (2 Hydroxypropyl) meth acrylamide (HPMA). Poly [N-(2-hydroxy)
meth acrylamide] (HPMA) is known as the first polymer for use
as a drug conjugate in pharmacy. For a long time, the use of
HPMA-based copolymers has been expanded multiple biomedical
applications. The copolymers of HPMA are used comprehensively
because of some special properties such as non-toxicity, high
hydrophilicity and non-immunogenicity. The conjunction of HPMA
with pharmaceutical compounds results in acceptable solubility in
water and the nanosized structure. Its various applications are con-
firmed in drug delivery because of its unique biological and physic-
ochemical properties [62].
Du et al. [102] used HPMA-PSf membranes for boron removal
with an efficiency of 62%. Schöttner et al. [103] fabricated PS-b-
HPMA membranes with pore diameters in the range of 20–
60 nm. According to the results, the surface of blended membranes
covered with irregular pores, looked like filaments. Wang et al.
[104] used HPMA in concrete to increase the retention factor. Liu
et al. [105] fabricated bisphosphonate-derived ligand membranes
that had hydrophilicity of HPMA and could also improve the flex-
ibility of the based polymer to have specific protein adsorption.
Koziolová et al. [106] studied the synthesis of the conjugation of
hydrophobic hexaleucine and a hydrophilic based one in the HPMA
Fig. 5. Porous membrane’s applications.
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
copolymer in cytostatic and antiviral drugs. Nuhn et al. [107] used
controlled radical polymerization and activated ester as a precur-
sor to synthesize HPMA-based copolymers. These kinds of HPMA
copolymers are multifunctional and obtain special potential for
use as a carrier for tumor immunotherapy. Stang et al. [108]
reported the synthesis of special polymeric membranes in the
composition of p(HPMA)-co-p(LMA), which led to effective incor-
poration of membrane proteins and prevented the hydrophobic
interplay of lipids and membranes.
Applications of pore formers
A wide range of applications including the pharmaceutical
industry, catalysts, waste and water treatment, and fuel cell
(Fig. 5) are defined schematically for the application of polymeric
pore formers and different methods for their participation in differ-
ent substrates such as phase inversion and plasma electrolytic oxi-
dation [14,109–111].
WSP are being used as additive to enhance the porosity and
hydrophilicity of polymeric membranes. Meng et al. [112] pre-
pared PVDF membranes by adding PEG as a pore former and
reported its great desalination property and consequently, the best
choice for application in water filtration. The hydrophilic nature of
PEG makes it a prominent choice for conjugating to hydrophobic
drug or carriers to have better solubility. Sarkar et al. [113] applied
polyamidoamine (PAMAM) dendrimers and PAMAM-PEG for fabri-
cating ultrafiltration membranes with better hydrophilicity. Better
antifouling property is another advantage of PEG incorporation in
water filtration. The non-toxicity of water-soluble polymers makes
them attractive additives in various biomedical and pharmaceuti-
cal applications. PVP-VA copolymers were used to improve the
poor solubility of some drugs, including indomethacin and nifedip-
ine [114,115]. Moreover, PVA was used in different biomedical
uses such as: catheters, hemodialysis, modification of soft tissue,
artificial pancreas, skin, and cartilage. PVA in the hydrogel manner
is also used in different biomedical and pharmaceutical industries
[116]. Special properties of these hydrogels such as bio-
adhesiveness, non-carcinogenicity and non-toxicity are the main
reasons to use them in various applications, including contact lens
formation, drug delivery and artificial heart lining[117]. A wide
range of applications is defined for PAA uses such as oral- and
mucosal- related applications (oral suspension, bio-adhesive and
controlling of drug release), an emulsifying agent for application
in low viscosity systems and a suspender for external applications.
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al. Journal of Industrial and Engineering Chemistry 109 (2022) 100–124

About the application of PAA drug delivery systems, the conjuga- increase in membrane ion exchange capacities leads to better-
tion of PAA with divinyl glycol yields a suitable bio-adhesive com- performing membranes and greater membrane swelling in water.
pound for related usage. Different kinds of FC are summarized in Fig. 6. The type of elec-
PEG copolymers have various uses in cardiovascular devices, trolytes is the main factor to classify the FCs.
especially in stunts because of their properties in decreasing For movable application, direct methanol fuel cells (DMFCs) are
agglomeration of the red blood cells and better amenability of studied as favorable power sources that have recently attracted
the blood. Furthermore, PEG copolymers have a special usage in many investigations. A slow rate of transformation is needed for
the formulation of hydrogels for chemical cross-linked and DMFCs. It should be noticed that, proton exchange membrane is
temperature-responsive applications. A temperature-responsive one of the main constituents of fuel cells, and perfluorinated poly-
system is an injection method for drug delivery systems [118]. mers (e.g. nafion Ò) are used exclusively as proton exchange mem-
The conjugation of different drugs/molecules (such as insulin, branes in direct methanol fuel cells in DMFCs.
lipids, daunmorubicine and camptothecin) with PEG was also stud- Among various kinds of Nafions that are known as commercial
ied previously [119]. items, the most applicable types are Nafions 112, 115, 117 and 110
The hydrophilic property of WSP results in comprehensive with the thicknesses of 50.8, 127, 177.8 and 254 mm, respectively.
usage in polymeric membranes due to more retention ability of They conduct protons highly and swell water slightly, however
water (usually at high temperature and light RHs) [120] and for thicker membranes are more useful for DMFCs. Despite the wide
application in fuel cells. PEG application is also reported in the
electrolytic field. A mixture of polyethylene glycol diacrylate oligo-
meric (PEGDME) and polyethylene glycol dimethyl ether (PEGDA)
with (CF3SO2)2N was identified as a suitable mixture for the elec-
trolyte of polymer. Ion conductivity (about 2.1  104 S cm1)
resulted in better mechanical and electrochemical properties, mak-
ing it suitable in power technology [121]. The high viscosity of oils
makes limits to their selective hydrogenation by usual hydrogenat-
ing techniques. Due to lower viscosities, however solvents were
added to the reaction media, and usual heterogeneous metal cat-
alyzers couldn’t work properly for hydrogenation. Metal dispersion
in a high value in the pores of polymeric membranes (carriers) is
the main solution to reach a large surface catalytic area. About edi-
ble oil (e.g. triglycerides of stearic acid), the slow diffusion of long-
chained compounds and the hydrogenation of double bonds take
place, but the obtained products block the pores of the catalysis.
For example, the mineralization of HA (hydroxyapatite) was done
by PEG-PAA-PCL with a corona structure and triblock copolymer
micelles [122]. In a similar study, different compounds of PVP
(PVP-Pd/CA and PVP/Pd/PAN) were used as hollow catalytic fibers
in reactors. The synthesized catalysis were also used for cyclopen-
tadiene hydrogenation [123,124]. Fritsch et al. [125] fabricated
PES- and PAI-based membranes with different contents of Pt to
hydrogenate about 50% of linoleic acid in catalytically reactive por-
ous membranes.

Proton exchangers

Proton exchange membrane fuel cells (PEMFCs) have shown the

potential to be commercialized as power sources in automotive,
electronic, portable, and stationary applications [126]. The mem-
brane electrode assembly (MEA), the heart of a PEMFC, is com-
posed of a membrane loaded with catalyst layers on each side
and is sandwiched between two porous layers named gas diffusion
layers (GDL). The applied pressure for sealing a PEMFC changes the
GDL thickness and porosity; affecting the transport properties of
the GDL.
Recently, fuel cells are considered widely because of their
important roles in transforming electrochemical energy. To know
more about fuel cell details, fuel such as hydrogen is donated to
the anode, while oxygen is donated to the cathode side. Electrons
are taken away from hydrogen atoms at the anode, and then the
generated protons go through an electrolyte that can conduct them
while electrons are conducted through an external pass to the
cathode, thereby reducing oxygen. Finally the protons are mixed
with oxygen making water and electricity [127].
The measurement of ion-exchange capacity allows the determi- Fig. 6. Summary of FC types. Polymer electrolyte membrane (PEM), direct
nation of the concentration of available conductive sites in a mem- methanol fuel cell (DMFC), alkaline fuel cell (AFC), phosphoric acid fuel cell (PAFC),
brane on a weight basis and may be readily tailored. Generally, an molten carbonate fuel cell (MCFC) and solid oxide fuel cell (SOFC).

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N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
use Nafions in industry, they have some serious disadvantages
such as i) high methanol permeability that decreases both fuel effi-
ciency and cell performance by rising the cathode over potential ii)
high price iii) not being a proper material for temperatures less
than 0 °C or higher than 100 °C, because water-filled channels
determine its proton conductivity. But, there are many advantages
to use fuel cells at high temperatures, and iv) their weak strength
at high temperatures [128–131]. The other previously noted disad-
vantages are especially the high cost, that encourages scientists to
develop new cheaper proton exchangers, and more stability in
chemical and mechanical features, especially at high and low tem-
peratures. Sometimes the performance of fuel cells in higher tem-
peratures provides more crucial advantages such as: reducing the
effect of CO in Pt-based catalyst poisoning, in other words, there
is no catalyst poisoning at temperatures higher than 160 °C
[130,132]. A large number of fluorinated solid polymer and non-
fluorinated electrolytes have been synthesized in recent years.
The proton conductivity mechanism of this kind of proton
exchange membrane is similar to NafionÒ, but the polymer poten-
tially has more advantages than NafionÒ due to the presence of
water therein. Some of their advantages and disadvantages can
be observed in the following part:
i) Polystyrene-based materials
The first commercial polymer membranes are polystyrene-
sulfonic acid membranes. The short life-time because of degrada-
tion decreases the interest in the development of these mem-
branes. However, a low cost of styrene-containing copolymers
and lower methanol permeability than NafionÒ attract some atten-
tion to their use [133,134]. It should be noted that the polystyrene-
sulfonic acid membrane material has considerably lower water
content and higher conductivity than NafionÒ too [135,136].
ii) Sulfonated polyimide-based (SPI) membranes
Polyimides are a kind of polymers that have high thermal and
mechanical stability as well as enough strength against harsh
chemical conditions [137–140]. In some cases, sulfonic acid
was used to modify it to obtain an improved hydrophilic prop-
erty for use as a proton conductor. Despite the low cost of
polyimide-based membranes, it was understood that swelling
against humidity is their main difficulty. To solve this problem,
hydration should be done to enable it for conducting protons
the same as NafionÒ. It is estimated as the main limitation to
their commercialization. The mentioned problem is the result
of the nucleophilic reaction between water and the neighboring
carbonyl group. Increasing electron densities at the carbon of
carbonyl groups can be a solution for drawbacks. Different
investigations were used to enhance imide vulnerability to
hydrolysis [141–144]. It should be mentioned that, the methanol
permeability of SPI-based membranes with the base of Sul-
fonated polyimide is really lower than NafionÒ for special pro-
cess conditions such as high temperature [145,146].
iii) Membranes based on polyphosphazene
Besides the low cost of polyphosphazene, the most valued char-
acteristic of this group of polymers, is its extreme stability of [-
n = p-] foundation against free-radical break reactions which
makes phosphazenes more suitable as a proton exchange mem-
brane in fuel cells [147,148].
The huge hydrophilicity of the [-n = p-] foundation reveals the
chance of using them in osmotic drug carriers with modest metha-
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
nol permeability. These characteristics as well as the elevated tem-
perature backbone stability, attract great notice for high
temperature FC and DMFC applications [149].
The most distinguishable feature in polyphosphaze-based
membranes is their low methanol permeability [133,150].
iv) Membranes based on polybenzimidazole (PBI)
PAFCs (phosphoric acid fuel cell) which are the design of a phos-
phoric acid FC, can be used at high temperature between 160 °C
and 220 °C. Applying high temperatures to their function changes
them to prominent items for industrial applications.
PAFCs as the membranes for conducting protons contain a
liquid-in-sponge matrix, which includes a thin silicon carbid
loaded with H3PO4 [151]. The liquid electrolyte can be noticed as
a drawback for PAFC and acts as an obstacle to its commercializa-
tion. Electrolyte leakage during the process and the necessity of
refilling during functioning [152], providing an acid tank for refill-
ing, and low thermal cyclability of usual PAFCs make them unsuit-
able for movable applications [153]. These problems attract the
growth of an enhanced matrix for H3PO4 as:
– Matrices in molecular-scales that soak a polymer using H3PO4.
In this modification, mechanism of the maintaining acid is the
chemical-type interaction.
– Macro-porous matrices use capillary forces to maintain acid.
– Some matrixes are polymers with chain holding basic sites, for
example: alcohol, ethers, imines, and imides. These polymers
should have reactions with acid and play the role of proton
acceptors and make ion pairs.
Among many investigations about polymers, PBI-based materi-
als, are the most suitable items for fuel cell membranes because of
their thermal and mechanical strength at elevated-temperatures
[154,155]. Fig. 7 shows the schematic of the PBI/H3PO4 poly salt
conduct proton. In this kind of poly salt H3PO4, the applied content
of poly salt should be used optimally to reach enough membrane
activity and strength [156]. This figure shows the two possible
ways for proton transfer: path A is actually the path of [(benzimi-
dazol ring) ⇨ (phosphoric acid)] and path B is proton transfer via a
chain of phosphoric acid molecules.
Some studies such as a linear PBI polymer and its cross-linking
were done to improve both conductivity and mechanical quality at
the same time [157,158]. High acid doping levels resulted in
enhance mechanical strength which was done by modifying the
main PBI chain random copolymers [159] and moderately fluori-
nated PBI membranes [160].
v) Another category of proton conductors is sulfonated pol-
yarylene ethers and sulfonated PEEK, which are used in fuel
cells as prominent ones [161–163].
High thermal and chemical stability and low cost are the main
features of this category. The ability of sulfonated polyarylene
ethers in proton conductivity reach to the fuel cell at high level
of sulfonation. Some developments have been done for preparing
this kind of membrane with fair conductivity [162,164,165]. More-
over, sulfonated PEEK with good conductivities of more than 0.1 S/
cm were studied, as well [166]. Scientists try to modify sulfonated
polyarylene ethers to achieve their better properties [140]. Cross-
linking processes are suitable for utilizing in medium and high-
temperature fuel cells [167,168].
Some cross-linker and cross-linking techniques have been
reported To obtain better properties of sulfonated PEEK [169].
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al. Journal of Industrial and Engineering Chemistry 109 (2022) 100–124

Fig. 7. Proton conductivity of [PBI/H3PO4] poly salt.

Fig. 8. Conductivity and water uptake of SPAEK and c-SPAEK membrane in different temperatures [167].

110
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
Fig. 8 shows the possibility to prepare a proton conductor that con-
ducts highly and absorbs water moderately [167].
Other methods such as combining polyaryl ethers with polymer
or mixing with inorganic fillers in the matrix of membranes are
usual ways to improve their properties [170,171].
vi) Nowadays, natural are environmentally friendly polymers
are widely synthesized to replace the synthetic ones in
application of fuel cells [172]. Cellulose and its derivatives
as a category of natural polymers were studied comprehen-
sively [173–175].
Chitosan (CS) can be named as another environmentally
friendly conductor. Although, membranes based on CS have low
conductivity [151,152,176], having considerably lower methanol
permeability than NafionÒ makes them more usable. To develop
CS-based proton exchange membranes, blending with poly(92-ac
rylamido-2-methylpropane sulfunic acid) is more familiar.
Gas solubility agents
During recent decades, polymeric membranes have attracted
special attention in different aspects of gas separation such as
hydrogen recovery and purification as well as carbon dioxide
(CO2) capture. The incorporation of polymeric additives into the
skeleton of the membrane matrix has several advantages to inor-
ganic additives, e.g. good processability, chemical stability and
low price [177]. About non-porous gas separation membranes,
gas transport performance is defined as permeability and selectiv-
ity. Nonetheless, it was confirmed that there is an interchange rela-
tionship between permeability and selectivity which was reported
in the title of ‘‘upper bound” by Robeson (1991) and explained the-
oretically by Freeman [178,179].
High selectivity and permeability are the main reasons to use
new polymeric membranes in industrial applications. Chemically
modified polymers and blending polymers are newly designed
methods to have block polymers. New materials with enhanced
properties are obtained by mixing two or more polymers, which
is a less costly method [180].
Between various polymeric materials, polyurethanes (PU) are
the group of copolymers divided into soft (polyol) and hard (urea
and urethane groups) segments [181]. High gas permeability is
the special property of this group of polymers to make them suit-
able choices for gas separation, especially for the separation of
polar components such as acid gases (e.g., CO2, and H2S) from
non-polar gases (e.g., CH4, N2 and H2). Different properties of PU
such as length, and the amount and type of soft and hard segments
can influence the performance of prepared membranes. For exam-
ple, the type of chain extenders used in the synthesis of PU affected
the permeability of fabricated membranes and, consequently,
changed the density, glass transition, crystallinity and morphology
of membranes [181]. Sales et al. [182] used polymethyl methacry-
late (PMMA)/PU blend polymers and investigated their gas separa-
tion properties. PMMA addition to the polymeric matrix decreased
the free volume of the flexible PU, and then decreased the gas per-
meability. It seems that the permeability to CO2 and H2 is corre-
lated with the average free-volume size. On the other hand, the
formation of the PU/PMMA blend improves membrane selectivity
of the small H2 molecule, which is probably associated with the
phase arrangement induced by the vitreous component.
PEBA (polyether-block-amide) membranes are strongly recom-
mended for the separation of polar/non-polar gas pairs e.g., CO2/N2,
SO2/N2 or CO2/H2, [183,184]. Chen et al. [185] reported that PEBA
2533 was one of the best choices for highly permeable to light
hydrocarbons. Permeation properties obtained with propane and
propylene indicated strong plasticization effects on the PEBAX
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
2533 polymer matrix. Nitrogen showed little interaction with the
membrane material, which is considered ideal. The permeability
of propane and propylene was strongly affected by both operating
temperature and feed pressure. The permeability of propane and
propylene increased with increasing pressure.
Car et al. [186] used PEG as an additive to the matrix of
polyamide-b-ethylene oxide (PebaxÒ) membranes and observed
two-fold growth in the permeability of the blend membrane by
the addition of PEG in 50% compared to pristine Pebax. Mixed
gas (CO2/H2, CO2/N2 and CO2/CH4) permeabilities were also per-
formed at different total feed pressures (fugacities), and the CO2
flux slightly varied for each binary mixture. Nevertheless,
PebaxÒ/PEG (50 wt.% of PEG) always presented the highest CO2 flux
and high selectivity, especially for CO2/H2.
In a similar study, a great improvement was observed in CO2
solubility due to PEG addition and the probable increase of the
fractional free volume because of adding EO units [187].
Mozaffari et al. [188] used a combination of PU and PEBA as a
blend membrane for gas separation. They applied the mixed fabri-
cated membranes for the separation of the gas composition (N2, O2,
CO2, and CH4). According to their observation, PU/PEBA blend
membranes are in the miscible category and more amounts of
PEBA in PU/PEBA in blending membranes, resulted in lower perme-
ability and higher selectivity for all of selected gases. Besides, the
obtained results indicated that, significant decrease in gas perme-
ability of membranes by adding PEBA to the PU membranes
occurred, which was attributed to the higher crystallinity of PEBA
and less phase separation between its soft and hard segments. The
observed trend for the permeability of the investigated gases in
blend membranes was as follows:
P (CO2 ) > P (CH4 ) > P (O2 ) > P (N2 )
The role of polymeric additives in gas separation membranes
In recent decades, several types of polymeric materials have
been applied to fabricate gas separation membranes. Moreover,
numerous investigations have been done to obtain improved
membranes with better morphology and structure and conse-
quently increase the performance of membranes in gas separation
from the experimental scale to module designs [189,190].
The performance of membranes may improve by the synthesis
of polymers with reforming structures. However, two unavoidable
parameters to use new synthetic structures on large scales are high
costs and the development period of polymers. To minimize the
risk of cost and duration, a feasible strategy to improve the separa-
tion performance is to modify the of present membrane materials.
About membrane for gas separation, a mutual reverse relationship
between high permeability and low selectivity should be consid-
ered in the modification [191]. Polymer blending [192], cross-
linking [193], and mixed matrix membranes (MMM) are the main
strategies that have been applied to modify and improve the exist-
ing membranes.
Symmetric and asymmetric formats can be used in gas separa-
tion membranes. Increasing flux and less consumption of expen-
sive materials lead to the fabrication of asymmetric membranes
with ‘‘thin-film composite (TFC)” structure. The typical composi-
tion of TFC membranes is a thin active layer with an extremely per-
meable gutter layer, which is later coated with the thin active
layer. However, the main limitation of TFC membranes is to pre-
pare the active layer with a special thickness and to avoid making
defects in the final composite structure [194]. Defect-free polymer/
inorganic particle interface, preparing uniform membrane mor-
phology, and separation performance are the main reasons for
the restricted fabrication of MMMs. Nevertheless, applying soft
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
Fig. 9. Schematic of adding the most applicable polymeric additives for gas separation.
polymers can be preferred as the alternative choice with the same
concept [195]. To overcome the shortcoming of membrane compo-
nents, polymer blending is the prominent method due to combin-
ing the effective properties of different components to make a new
composition with a specific target. Cost-effectiveness, simplicity,
and reproducibility are the special properties of the polymer
blending method. Miscibility of blending at the molecular level is
the main limitation of polymer blending, thus, being the major dis-
advantage of the polymer blending modification method.
Furthermore, plasticizing polymers is very common in gas sep-
aration membranes, and blending with a less plasticizable polymer
reduces this defect. The transportation of a specific gas can be facil-
itated by applying an appropriate polymer in the primary poly-
meric matrix. This review is focused on the recent blending
membranes and their performance in the terms of selectivity and
permeability. Fig. 9 shows the most common polymeric additives
used in polymeric membranes for gas separation.
PEG additive
The most generally studied polymeric additive to obtain the
better performance of polymeric gas separation membranes is
PEG in PebaxÒ [196]. The polar ether group in the PEG structure
is the main reason for its tendency to separate polar CO2 gas in
the mixture of different gases. In addition, better mechanical
strength is another advantage of blending PEG in the polymeric
matrix. Car et al. [186] applied low-molecular-weight PEG to
improve the PebaxÒ membrane for better separation in the mix-
ture of H2, N2, CH4, and CO2. A blended membrane with 50% PEG
made an improvement about two times in the permeability of
CO2 to pure PebaxÒ, which was attributed to ethylene oxide and
better solubility of CO2 in the modified rubbery polymers.
Although, no significant changes were observed in the mixture of
CO2/N2 and CO2/CH4 because of the same growth of CH4 and N2
permeability to CO2 and eventually the selectivity was maintained
therein. PEG addition improved a micro phase-separated structure
and decreased the crystallinity of PebaxÒ membranes. In another
study [187], the effects of temperature and pressure were tested
on the PebaxÒ/PEG blend TFC membranes. Pressure variations up
to 20 bar and a temperature range of 283–333 K were applied to
single gases and CO2/H2, CO2/N2 and CO2/CH4 mixtures. The study
showed an Arrhenius-type relationship between the temperature
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
and permeation of blend membranes. The same behavior was also
observed with higher pressure and permeation about single and
mixed gases. Yave et al. [197] investigated an interesting example
of a blend membrane. PEG-dimethyl ether (PEG-DME) was used in
the polymeric matrix of PebaxÒ to fabricate nanostructured thin-
film membranes for the separation of CO2. The blend membrane
showed more mechanical stability than the pure one and increased
the CO2 permeability about eight-fold.
Reijerkerk et al. [198] used the same polymeric matrix and PEG-
polydimethylsiloxane (PDMS) as an additive. PebaxÒ/PEG-PDMS
with high loading of PEG-PDMS showed a high improvement of
CO2 permeability (about 500%), but no significant changes were
observed in the selectivity of gas mixtures.
Hu et al. [199] applied the same combination of PEG-PDMS as a
copolymer in poly(2,6-dimethyl-1,4-phenylene oxide) (PPO) and
used the phase inversion technique for the asymmetric membrane
fabrication applied for CO2 separation. The CO2 permeability of
blend membranes with 40% PEG and 50% PEG-PDMS improved four
and five times relative to the pure PPO membrane, respectively.
The permeability of CO2 and CO2/N2 selectivity of the blend mem-
brane increased under higher pressure. This growth defined that
increased membrane porosity and a thinner skin layer were the
results of additives.
Polyurethane additive
Polyurethane (PU) is one of the prominent polymers in the class
of elastomeric and applicable as membrane material classified into
soft and hard structures, which are phase-separated. Good
membrane-forming ability and increase permeability are two pos-
itive properties of PU membranes; however, the selectivity of PU
membranes is not attractive. Therefore, it should be blended with
highly selective polymers to prepare slightly gas separation mem-
branes. Patrício et al. [181] fabricated PU/PMMA blend membranes
in different contents and studied the separation of H2, N2, O2, CH4,
and CO2 gases. The probable hydrogen band interaction between
PMMA and PU resulted in PMMA as the dispersed phase and PU
as the continuous phase for the blend membranes. By increasing
PMMA content in the matrix, the permeability dropped due to
the smaller free volume size, but the selectivity of H2/N2 increased
because of creating a more rigid amorphous phase. The pressure of
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
feed didn’t significantly affect the permeability and selectivity of
blend membranes.
Kim et al. [200] fabricated PU/PEI and PU/Polyamideimide blend
membranes to investigated their morphology and CO2 permeabil-
ity. In addition to microphase separation, an increase in selectivity
and a decrease in permeability were observed due to lower con-
tents of PU and an increase in the volume fraction. Semsarzadeh
et al. [201] prepared PU/polyvinyl acetate (PU/PVAc) blend mem-
branes with and without adding polyethylene oxide–polypropy-
lene oxide–polyethylene oxide triblock copolymer (PluronicÒ) for
the transportation of N2, O2, CH4, and CO2 gases. The hydrogen
bonding interaction between PVAc and PU polymers resulted in
heterogeneous blends. The compatibility of blends increased due
to the block copolymer addition. The polar nature of PVAc and
CO2 gas caused an improvement in permeability even in the small
addition of PVAc contents. About other gases, the increase of PVAc
contents changed the structure from amorphous to crystalline and,
eventually, reduced permeability during the separation process.
Using co-polymer didn’t significantly affect the properties of mem-
branes such as gas transport. For the mixture of CO2/N2 gases, good
separation was observed close to the Robeson line [202].
Polyimide (PI) additive
Very low plasticization resistance and very low permeability
are the main reasons to use PI as a blending polymer. Other prop-
erties of PI, such as great thermal and mechanical stabilities, high
selectivity, and glass transition temperature make it a prominent
choice for blending in gas separation membranes [203]. About
the blending matrix, to gain superior mechanical, thermal and
gas separation properties, PI should be blended with special poly-
mers with high permeability and plasticization resistance. How-
ever, the low thermal and mechanical stability of the base
polymer is not important. Different kinds of membranes, such as
hollow-fiber, dense, asymmetric, and mixed matrix membranes
(MMMs) were used for the PI blending test. Khan et al. [202] incor-
porated PI (MatrimidÒ 9725) in the matrix of sulfonated PEEK (S-
PEEK) in any possible composition range and observed perfect mis-
cibility over all ranges. The increased permeability of CH4, CO2 and
N2 gases resulted in higher contents of the S-PEEK polymer but no
significant changes were observed in selectivity. Induced plasti-
cization made an improvement in the CO2 permeation of mixed-
gas separation at higher pressures. Better plasticization resistance
can be achieved at a higher concentration of S-PEEK with higher
pressures. At higher temperatures, the gas permeability and selec-
tivity increased and decreased, respectively, due to the flexibility of
polymer chains. The plasticization resistance of blended mem-
branes usually improve due to chemical cross-linking modification
up to 40 bar pressure, but the separation efficiency faced negative
effects.
About hydrogen purification, Hosseini et al. [204] applied
blending and chemical cross-linking modification for the Matri-
midÒ 5218/PBI miscible blend for the separation of CH4, N2, CO2
and H2 gases. The separation performance of dense blend mem-
brane was excellent for H2. A higher PBI content reduced gas per-
meability as a result of a lower (FFV). Better chain packing with a
higher PBI concentration makes a significant improvement in the
selectivity of H2/CO2 and H2/N2 pairs. About the H2/CO2 pair, the
selectivity growth of cross-linked MatrimidÒ blend membranes
was from 3.88 to 26.09. Moreover, the effect of chemical cross-
linking on the gas permeability decay of membranes is probably
due to the tighter interstitial spaces among the chains and restric-
tion in the vibration and mobility of polymer chains and side
groups attached to the backbone.
Young et al. [205] fabricated MatrimidÒ-rich membranes and
used them for CO2/CH4 separation. All the blend membranes exhib-
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
ited a considerable improvement in gas permeability and a little
decrease in selectivity while all of them were below the upper
bound.
There are also reports on asymmetric blend membranes and
using the phase-inversion method. Han et al. [206] separated a
mixture of O2/N2 gases by fabricating PES/PI (MatrimidÒ 5218)
blend membranes. All membranes in the higher feed pressure
showed increasing permeability. However, increasing pressure
reduced the O2/N2 selectivity from 5.4 to 4.9. Totally, polymer
blending changed the stability of membranes and made them more
resistant under harsh conditions especially in pressure and tem-
perature levels.
Accordingly, polymer blending as a modification method is
known as a time- and cost-effective technique to make improve-
ments in the thermal, mechanical, and separation performance of
gas separation membranes. PIs, Pus, and PEGs are most commonly
applied in blend membranes.
The role of polymeric additives in liquid filtration membranes
The structural pore morphology of polymeric membranes can
be controlled during their preparation. Organic polymers are the
most applicable because of their flexibility, permeability and abil-
ity to form diverse structures. Various methods that are used to
prepare this kind of membrane include phase inversion methods,
track etching, nanolithography-microlithography, template leach-
ing, sintering, stretching, template leaching, interfacial polymer-
ization and spinning [207].
More explanation about the phase inversion and interfacial
polymerization can be found below due to the numerous uses of
these two methods:
Phase inversion membranes
In the phase inversion process, a polymer melt/dope from the
liquid phase is converted to the solid phase through a controlled
route. Usually, four methods are used in the phase inversion
method: 1) NIPS: non-solvent induced phase inversion, 2) TIPS:
thermally induced phase separation, 3) EIPS: solvent evaporation
induced phase separation and 4) VIPS: vapor induced phase
separation.
In the NIPS method, a suitable solvent, such as CA, PSf, PVDF and
PES, is selected for solubilizing some polymers. A thick film (about
50–200 mm) of polymeric solution is deposited on a fabric or glass
support, and then drawn into a non-solvent bath of water for coag-
ulation. Symmetric or asymmetric membranes will form because
of the polymer solution coagulation in phases with solid
polymer-rich and liquid solvent-rich phases [208].
The TIPS method is usually used to fabricate membranes in
which the applied polymers can’t easily dissolved in a solvent at
low temperature. In this method, a polymer such as polypropylene
(PP) or polyethylene (PE) dissolves in an appropriate solvent at
high temperatures. Then, cooling process causes to precipitate
the polymer. After complete precipitation, different methods such
as extraction, evaporation or freezing, are used to extract solvent.
Thermodynamic parameters including temperature, temperature
reduction rate, the concentration of polymer dope, and the solvent
system, are the main factors to control the pore size of the asym-
metric membrane [209].
In the EIPS method, two or more volatile solvents with different
boiling points and dissolution capacities are used to make a homo-
geneous polymeric solution with special polymers (PVC, PVAc and
polystyrene). Eventually, the homogeneous polymeric solution
spread-out to prepare the membrane in the form of a thin film.
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
In VIPS, the vapor of non-solvent (such as water) will expose to
a spread polymeric solution. In the next step, its absorption onto
the cast dope solution precipitates the polymer as a solid- phase
membrane [207]. Some parameters such as polymer concentration,
solvent type, non-solvent type, coagulation bath temperature, etc.,
as well as polymeric additives in the casting solution can affect the
morphology, chemico-mechanical, and pore size of the synthesized
membranes [210].
Some additives with low or high molecular weights are used in
the cast solution to improve the morphology and performance of
the phase inversion-induced membranes. Additives such as organic
or inorganic components can provide a spongy membrane and
increase pore formation and pore interconnectivity, which conse-
quently results in improved hydrophilicity.
The majority of investigations are focused on all-purpose poly-
meric additives such as PVP, PEG and PEO and their effect through
the phase inversion method [74,211,212].
About PVP, for example, Boom et al. investigated the PVP role in
the preparation of PES in NMP solvent. They understood that PVP
addition could help the formation of macrovoid pores [213]. The
hydrophilic property of the membrane can be changed by solving
PVP in its polymeric solution [214]. Numerous studies also investi-
gated the effect of various molecular weights of PVP [215,216] and
its concentration on the membrane properties such as its morphol-
ogy and function [217–219].
PSF membranes were synthesized by adding PVP as a high
molecular weight polymeric additive and a demixing enhancer
through the phase inversion method. Adding the PVP additive,
speeds up the phase separation of the polymeric casting solution.
Moreover, enlarged the macrovoid structure of the membrane
pores. Adding a permeate flux of about 20 times to the prepared
membrane without PVP is another result of changing the pore type
of blend membranes. This claim has also been confirmed in other
studies [37,38,74,211,212,220–222].
PEG is another polymeric additive that plays an important role
in the pore-forming of liquid filtration membranes and is used
through the phase-inversion method. Different studies investi-
gated the effect of a polymeric additive with different molecular
weights [223–225] and concentrations [226,227]
Kim et al. investigated the effect of PEG on the thermodynamical
and precipitation kinetics properties of synthesized membranes by
viscosity, coagulation value and light transmittance measurements.
Less stability in the thermodynamic property of membranes was the
result of increasing the ratio of PEG to polymer content to the
selected solvent or applying PEG with a higher molecular weight
[223]. It was also observed that using PEG resulted in bigger pore
size, a more porous top-layer, and, consequently, higher water flux
content and lower solute rejection. Moreover, more porosity in the
top-layer needs to have more distance from the starting point of
macrovoids to prevent non-solvent to the sub-layer. Large amounts
of non-solvent inflow result in nuclei formation and limit macrovoid
formation. It should be noted that the hydrophilic property of PEG
could help to improve the permeability of fabricated membranes
by causing pores on them [228].
Another study examined the effect of different kinds of PEG
molecular weights on the synthesis of PEI asymmetric membranes
[229]. Using PEG200 in the casting solution of PEI/NMP decreased
the coagulation value and increased the polymeric solution viscos-
ity. Adding PEG200 resulted in the ability of the polymeric solution
to approach the incipient-phase separation point and faster thin
film formation during the dry-phase inversion method. Therefore,
PEG200 is one of the suitable non-solvent additives to fabricate
asymmetric membranes with macrovoid-free sponge support layer
with a dense skin layer.
Zheng et al. [230] discovered that PEG could affect PSF solution
thermodynamically and rheologically. They studied the effect of
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
the bath temperature and PSF concentrations. At a specific temper-
ature, upward and downward trends were observed respectively,
about kinetics parameters of the membrane formation as PEG con-
tent increased from 4 to 16% wt%. Mei et al. [212] used the phase
inversion method by three additives (PEG, PVP, and sucrose) to fab-
ricate asymmetric PVC microporous membranes. They observed
that the viscosity of PVC/additive/DMAc membranes increased sig-
nificantly to the PVC/DMAc membrane. Three different additives
affected the gelatin velocity on thermodynamic process in the
sequence of PVP > PEG > sucrose. It was concluded that the modi-
fication of thermodynamic and kinetic properties due to participat-
ing the polymeric additive resulted in morphological and
structural change in blend membranes during phase inversion pro-
cess. However, the addition of small contents of sucrose signifi-
cantly, and changed the kinetic property and structure of
membranes to sponge-like, and the PVP addition mainly affected
larger finger-like pores from the top to the bottom of membranes
[212].
Oskoui et al. [231] investigated possible changes in the proper-
ties of nanolayered double hydroxide (NLDH)/PVDF nanocompos-
ite UF membrane by the addition of different hydrophilic
polymers, e.g., PVP and PEG (with different molecular weights)
and amphiphilic copolymers e.g. Pluronic F-127. According to their
observation, a special interaction happened between the polymeric
additives and NLDH nanolayers during the phase inversion process.
Moreover, the addition of PVP29000 at 1 wt.% highly affected dif-
ferent properties of blend membranes, including porosity,
hydrophilicity and cross-sectional morphology, as well as opera-
tional properties of NLDH/PVDF membranes. Farjami et al. [226]
used the same polymeric additives to the matrix of EPVC/boehmite
nanocomposite membranes. Unlike the previous study, the addi-
tion of PEG4000 in an optimum amount of 2 wt.% was the ideal
choice to reach the best morphological and operational properties
of EPVC/boehmite nanocomposite membranes. This shows that
performance of a polymeric additive in the membrane preparation
is also related to the host polymer chemistry.
Pagidi et al. [33] synthesized PSf membranes through the phase
inversion method. They used N-methyl-2-pyrrolidone (NMP) and
optimized its fouling resistance and permeation flux by participat-
ing simple hydrophilic polymeric additives such as PVP, PEI, PES
and PEG, as polymeric additives. A significant effect of polymeric
additives was observed in the limitation of concentration polariza-
tion at the gel layer on the surface of the membrane, which
resulted in reversible fouling in oil–water mixture separation.
Polyethylene terephthalate (PET) membrane were found to
have enough resistance to a wide range of solvents as well as chlo-
rine and acidic medium. Pulido et al. [232] synthesized porous
membranes of PET through the non-solvent-induced phase separa-
tion (NIPS). PET was obtained from water bottles, and PEG was
used as a polymeric additive and pore performing agent in differ-
ent contents. Finally, the produced membrane with an MWCO of
40 kg/mol in DMF was used in ultrafiltration at a high temperature
(100℃) and had suitable resistance against high chemical and heat
conditions.
Polydopamine (PDA) is one of the nano-sized spherical products
produced in the reaction media and adheres firmly on the sub-
strate when immersed in the solution for a specific duration. PDA
can cohere to most organic and inorganic substrates even with
non-adherent materials such as polytetrafluoroethylene (PTFE)
[233]. The special property of PDA attracted others attentions to
use it as coverage for nanomaterials including TiO2 NPs[234], gra-
phene [235] and clay [236] which enhances the interfacial interac-
tion between the polymeric matrix of membranes and inorganic
additives. According to the reports, the growth of interfacial inter-
action due to a combination of covalent and non-covalent interac-
tions such as hydrogen bonding interactions, p-stacking and
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
charge transfer, not only increased interfacial interactions but also
could provide the nanocomposite participation with new function-
alities because of the related properties of the bioinspired PDA
[237]. Jiang et al. [237] used bioinspired PDA NPs as additives in
the formation of PVDF membranes. According to their report, the
hydrophilicity of the blended membranes showed a significant
growth relative to the bare one. Furthermore, the PDA/PVDF blend
membranes developed stability for a long time in an aqueous
environment.
Among the group of polyimide polymers, Matrimid has been
used in a wide range as the parent polymer in polymer blend
because of high selectivity and thermal stability with a Tg of
320 °C. The strong hydrogen bonding interaction is the main rea-
son that results in a homogenous system such as Matrimid/Torlon
and Matrimid/P84 [238]. It should be mentioned that a compre-
hensive miscible system, which was confirmed by FTIR spectra, is
the result of hydrogen bonding between the –NH group or the
imide carbonyl group of Torlon, the –NH group in PBI and the car-
bonyl group of Matrimid.
However, Loloei et al. [239] presented that Matrimid could not
to form miscible blends with PEG. They reported that the forma-
tion of miscible blends was effectual in a low 3–5 wt% PEG and
were partially miscible blends in higher amount of 10–20 wt%
PEG in blend concentrations. In a similar study, Castro-Muñoz
et al. [240] studied Matrimid with the addition of PEG up to 5 wt
% for CO2/CH4 separation. Amazingly, the participation of PEG
resulted in a higher Tg, which could have resulted from the pres-
ence of more polar groups in the PEG structure and this modifica-
tion could increase the cohesive energy of the blends.
PVA is an aliphatic hydrophilic polymer with the presence of
the hydroxyl group and is widely used in membrane fabrication.
However, the crystalline structure of PVA yields a low flux and con-
sequently, meets the problem of membrane swelling in pervapora-
tion application. Yeom and Lee [241] performed one of the
attractive studies about the PVA/sodium alginate (SA) blend mem-
brane. They studied the compatibility of these two materials and
confirmed a fully compatible mixture despite having an opaque
manner when used in the phase inversion process. In another
study, it was concluded that the blend solution of PVA/CS was opti-
cally clear and phase separation was not observed after a long per-
iod at room temperature. The amount of swelling of the blend
membrane is directly related to higher water contact and signifi-
cantly increased by more water absorption [242]. It should be
mentioned that PVA is less noteworthy in gas separation than per-
vaporation due to its low permeability.
Klepić et al. [243] used a blend membrane of PVA and [EMIM]
[DCA] for CO2 separation. They reported that the diffusion-
Fig. 10. Interactions between cPIM-1 and Torlon (hydrogen bonding + charge transfer complexes (CTCs)) [249].
115
Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
controlled process was the ruling process in lower amounts of
[EMIM][DCA] content (less than 20 wt.%), while solubility-
controlled process played this role in higher amounts (more than
20 wt.%). The obtained permeability of blend membranes showed
significant growth in comparison to bare PVA. PVA/[EMIM][DCA]
in the portion of (47:53) yielded CO2 permeability in a high value
and more CO2/H2 selectivity which exceeded the Robeson upper
bound line.
Polymers of intrinsic microporosity (PIMs) are a group of porous
organic polymers which include voids in the microporous and con-
trolled structure, and were firstly reported by Budd et al. [244]. The
unique structure of PIMS exhibited conventional microporous
behavior and could be processed to a dense film, with great poten-
tial for use in membrane separation [245,246].
Generally, PIMs are known as prominent candidates in blending
polymers to make better permeability of a new blend compound.
Yong et al. [247] investigated the miscibility of blending PIM-1 (a
common derivate of the PIM group) with Matrimid in commercial
grade by a polar light microscope (PLM) [247]. They reported that
fully miscible and single phases were achieved using less than 10
wt.% Matrimid. More amount of Matrimid led to a partially misci-
ble phase with the existence of two phases at the same time. Hao
et al. [248] reported partially miscible of PIM-1 and poly[2,2-bis[4-
(3,4-dicarboxyphenoxy)phenyl]propane-m-phenylenediimine] or
polyetherimide (Ultem) in all blend ratios. Because of the ow solu-
bility of PIM-1 in special solvents, PIM-1 was modified to form car-
boxylated PIM-1 (cPIM-1) or hydrolyzed PIM-1 (hPIM-1) through
hydrolysis in a medium of sodium hydroxide, ethanol and water
to replace the nitrile groups with carboxylic acid groups. Due to
the modification, cPIM-1 and hPIM-1 dissolved in different polar
solvents. In a similar study, Yong et al. used modified cPIM-1 to
increase the polymer miscibility with Torlon (Fig. 10). Based on
their results, the addition of cPIM-1 up to 10 wt% led to single
phase and homogeneous blends [249]. Similarly, Salehian et al.
[250], used cPIM-1 at less than 10 wt% to form cPIM-1/P84 and
observed the miscible blends. Among different studies done by
research groups, the most compatible system belonged to cPIM-
1/Matrimid blends and the least one related to the PIM-1/Ultem
blend system. The blend system of PIM-1/Matrimid demonstrated
a miscible blend and a single phase at lower amounts of Matrimid
(i.e., 10 wt%) and were partially miscible at higher amounts [205].
Hydrogen bonding interactions and, consequently dipole–dipole
interactions are much stronger than physical interactions such as
charge transfer complexes (CTCs) Thus, the anticipation of hydro-
gen bonding joint with CTCs interactions resulted in better com-
patibility between cPIM-1/Matrimid than the PIM-1/Torlon
blends. Fig. 10 shows the schematic of this interaction.
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al. Journal of Industrial and Engineering Chemistry 109 (2022) 100–124

Table 2
Examples of some novel polymeric additives in modification of polymeric membranes.

Base Additive The effects of additive Ref.

polymer
PVDF Copolymer [(PVDF-co-CTFE)] Improving antifouling property [251]
PVDF-co- PEG and LiCl – PVDF-co-CTFE showed better performance than the PVDF [252]
CTFE – Increasing pore size and porosity
PVDF PVDF-co-CTFE PVDF-CTFE copolymerization membrane was better than PVDF/CTFE blending [253]
membrane
PVDF Copolymer [PS-b-PEGMA] Improving porosity and antifouling property [254]
PVDF Polystyrene-b-PEG Lower biofouling [254]
PVDF PVP Larger finger-like porosity with higher mean pore size [255,256]
PVDF PSF Improving mechanical properties of permeability [257]
PVDF PEG Higher pure water flux [258,259]
PES Copolymer [PDMS-PED-PPO-PEO-PDMS] Preparing amphiphilic surface with fouling-resistance [260]
PES Copolymer [P(PEG-r-PDMS)] Low-fouling UF membrane [261]
PES Copolymer [MPC], [BMA] Antifouling property [262]
PES Pluronic copolymers with different MW Improving pore size and porosity [263]
PES Polyimide – Improved ethylene permeability [264]
– Enhanced ethylene/N2 selectivity
PSf SiO2/PDA Smoother surface, increasing hydrophilicity and removing Cr(IV) [265]
PSf Hyperbranched polyethyleneimine functionalized Improving permeability, dye removal and antifouling property [266]
SiO2/PVP
PSf Sulfobetaine polyimides (three different MW) Enhancing permeability, antifouling and protein rejection [267]
PSf PSF-b-PEG – Additive causes larger pore size and narrower pore size distribution [268]
– Improved permeability and antifouling properties
PVA PVP Generating more compact structure by blocking interspatial cavities in top layer [269]
Nafion Sulfonated organosilicon dendrimers Improving ion exchange capacity and water retention capability [270]
PAN PEG Hydrophilicity, antifouling property [271]
PAN PAN-g-PEO Protein antifouling property [272]
PAN Zwitterionic copolymer Antifouling property [273]
PVC PVC-g-PEGMA Hydrophilicity, antifouling [274]
PVC Polyethylenimine functionalized halloysite nanotube/ Improving permeability, dye removal and antifouling property [275]
PEG
PVC Pluronic F127 Improving hydrophilicity, permeability and antifouling property [276]
CA Thiazole-based polyimine – Improved CO2 permeability [277]
– Enhanced CO2/N2 and CO2/CH4 selectivity

PEGMA: polyethylene glycol methacrylate; CTFE: chlorotrifluoroethylene; PAN: polyacrylonitrile; MPC: 2-methacryloyloxyethylphosphorylcholine; BMA: n-butyl
methacrylate.

Table 2 presents some studies briefly, which used polymeric
additive in the main polymer matrix to improve their
properties.
Interfacial polymerization (IP) membranes
The most important method for the commercial fabrication of
thin-film composite (TFC) membranes is interfacial polymeriza-
tion. Cadotte et al. [278] used the IP method to fabricate TFC mem-
branes for the first time. This membrane consists of two district
layers, the support layer is a kind of polymeric membrane prepared
mostly through the phase inversion method and the second one is
an ultra-thin skin layer. Different kinds of polymers can be used in
these two layers and each layer can be modified separately. Some
parameters such as the concentration of monomers, the type of
solvents, the time of reactions, and the construction of the barrier
membrane layer, influence the structure and morphology of syn-
thesized TFC membranes.
In the IP process, a polymer can be replaced with one of the
monomeric reagents.
Besides, new monomers for interfacial polymerization [279],
new active organic modifiers in trimesoyl chloride (TMC), or m-
phenylenediamine (MPD) solutions, were used to improve the IP
process [280].
Using a suitable UF support is very crucial, because its morphol-
ogy, pore size, and chemistry, can influence the morphology and
property of the final composite [281]. Furthermore, other parame-
ters, such as the thickness of the top layer, the chemistry of the sur-
face, reactants, kinetics of reaction, the time of reactions, and
additives can influence the final properties.
PEG is one of the prominent polymeric additives used to
improve the formation of the top layer of TFC membranes. In the
aqueous phase, PEG can be used as a wetting agent to improve
the hydrophilicity of PSf UF support membranes.
Jimenez-Solomon et al. [282] described the fabrication of a new
generation of organic solvent nanofiltration (OSN) membranes. The
IP technique and solvent activation were used to fabricate TFC
membranes in high flux. The resulting TFC membrane showed sig-
nificantly higher permeability for different polar aprotic solvents
such as DMF, acetone, and THF. The applied support for the fabri-
cation of these TFC membranes was cross-linked polyimide (PI)
UF membranes, which are solvent-stable. In this research, PEG
was used to impregnate the UF support due to the increased sol-
vent flux. Consequently, a PEG-impregnated support layer resulted
in increased fluxes in comparison to UF supports without PEG. To
improve TFC membranes, the second method was an ‘‘activating
solvent” after the IP reaction. This kind of treatment improved sol-
vent fluxes without a significant change in rejection. Therefore, IP
and using an activating solvent for treatment could lead to the next
generation of high-permeability OSN membranes.
Ghosh et al. [283] comprised six different composite mem-
branes consisting of PSf with different polymeric additives (PEG-
8k, PVP-8k, and PVP-40k) as supports which were prepared
through the phase inversion method and PA as the active layer of
TFC membranes. The PA layer on the hydrophilic support mem-
branes prepared by the addition of the mentioned additives was
slightly thinner, smoother, and less permeable. It is expected that
thicker TFC layers are less dense and consequently more perme-
able. The PEG-8k support had the most hydrophilicity but the low-
est permeability. They concluded that larger pores and

116
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
hydrophobic skin layers caused rougher and more permeable com-
posite membranes. The main reason for this phenomenon is the
hydrophobic nature of the applied support. The hydrophobic sup-
port doesn’t allow MPD molecules to permeate through the sup-
port and, consequently, a thin layer of PA is formed on the
support surface [283].
Wang et al. [284] used the IP reaction on porous polymeric sup-
ports to prepare high-performance forward osmosis (FO) mem-
branes. They used the in-situ polycondensation reaction to
prepare a thin aromatic PA selective layer with a thickness of
150 nm using p-phenylenediamine and 1,3,5-trimesoylchloride
as monomers on the PES/sulfonated PSf (SPSf)-alloyed porous
membranes. The modified FO membrane exhibited a higher flux
of the NaCl solution relative to unmodified membranes [284].
The polymeric additives could be added to IP monomer solu-
tions to modify the formed PA layer. Chae and Kim [280] enhanced
the permeability of a piperazine (PIP)-based TFC membrane by
roughening its smooth surface using highly organic-soluble addi-
tives (PEG with different molecular weights, PVA and diallyl phtha-
late) added to the PIP-aqueous solution. The hydrophilic additives
could quickly diffuse into the TMC organic solution promoting the
diffuse of PIP during the IP reaction, and consequently, causing to
an enlargement in the number and size of ridges on the fabricated
TFC membrane surface. Among the tested additives, the PEG was
the most effective one, and PEG with lower MW presented a better
influence. The membranes fabricated with PEG2000 and PEG200
showed 9 and 41% improved flux in comparison to the bare mem-
brane, respectively, in spite of their comparable hydrophilicity.
Asempour et al. [285] synthesized a new thin film nanocompos-
ite (TFN) by embedding different amounts of cellulose nanocrystals
(CNCs) into the PA layer. The modified membranes showed
improved hydrophilicity and pure water flux. Moreover, CNCs-
based TFN membranes are inexpensive and these properties make
it a candidate as a prominent option for large-scale usage in water
desalination. It should be noted that the possible leaching out of
CNCs is environmentally friendly and doesn’t lead to health and
environmental concerns.
Wang et al. [286] synthesized an aminophend/formaldehyde
resin polymeric nanosphere (APFNS) and applied as a polymeric
additive into the PA layer of TFC RO membranes. The hydrophilic
APFNS is rich in amino and hydroxyl groups because of using 3-
aminophenol monomer in the synthesis reaction that can chemi-
cally bond to the PA layer due to reacting with TMC. The mem-
brane modified by APFNS presented a flux of 71.3 L/m2h (two
times of the unmodified TFC membrane) with similar salt rejection
(96%). In addition, the polymeric nanosphere modified membrane
exhibited admirable chlorine resistance and antifouling
performances.
In another related article, an engineered NF membrane was syn-
thesized via the zwitterionic copolymer [287]. The single-step free-
radical polymerization between 2-methacryloyloxyethyl phospho-
ryphorylcholine (MPC) and 2-aminoethyl methacrylate hydrochlo-
ride (AEMA) was used for the synthesis of the copolymer. High
performance NF membrane with favorable rejection was fabricated
by the PA and the copolymer P[MPC-co-AEMA].
The role of polymeric additives in ion-exchange membranes
An ion-exchange membrane is known as the heart of electro-
dialysis which is the electrochemical separation technology for
separating inorganic salts and organic ionic species [288,289].
According to the kinds of ions that are allowed to pass through
membranes, ion-exchange membranes are divided into two main
categories: cation exchange membrane (CEM) and anion exchange
membrane (AEM). The AEM allows an anion to pass through layers
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
but resist against cations. Ion-exchange membranes are exten-
sively used in industrial processes that need to separate ions,
including food industries, desalination and fuel cells to recover
valuable species [290].
A comprehensive review is available on the development of ion-
exchange membranes used in capacitive deionization membranes
due to the importance of desalination [291].
Some additives are used to enhance ion-exchange membrane
properties. Among various additives, our focus is on polymeric
additives used to modify polymeric ion-exchange membrane.
Polyaniline (PANI) is a polymer with great electric conductivity
and electrochemical versatility. PANI has great reactions against
guest molecules at room temperature and enough ability to shape
in different structures and morphology such as thin films or nano-
fibers. This polymer is used as a base or an additive for ion-
exchange membrane [292]. In 1996, Nafion doped polyaniline
was reported in point of examining its conductive characteristics
[293].
The PANI is known to have high H+-selectivity and can dissolve
easily in various organic solvents with functionalized organic acids.
Therefore, PANI is a prominent component to be used as an H+-
sensitive additive. Lindfors et al. used a mixture of various amounts
of PANI as the H+-sensitive in plasticized PVC to study their pH and
redox sensitivity [294]. The pH sensitivity varied between pH 2 and
9. It was observed that the hysteresis effect of pure PANI could be
decreased by participating the appropriate amounts of plasticized
PVC. Svetlana et al. found a condition that was needed to make a
composite consisting of an anion-exchange layer of PANI on the
hydrophobic non-porous film of PTFE (F-4SF). They used various
organic solvents for the pretreatment of F-4SF in the synthesis pro-
cess. Finally, the synthesized ion-exchange composition was com-
pletely pH-sensitive because of the protonation–deprotonation
reaction of the emeraldine salt. Moreover, they studied surface
morphology, optical, and sensor characterizations as well as the
position of PANI on the surface of the polymer. Furthermore, this
modification is reversible for the chemical structure of PANI, there-
fore, the synthetic composite F-4SF/PANI can be applied for the
growth of optical pH sensors [295]. Melnikov et al. [296] prepared
three kinds of ion-exchange composites on the Ralex AMH mem-
brane (a heterogeneous ion-exchange membrane was chosen as
the substrate-membrane). as the base:
1) Deposite perflurocarbon cation-exchanger on the Ralex
membrane (bilayered composition)
2) Polyaniline and Ralex membrane composition (bilayered
composition)
3) Perfluororocarbon-PANI-Ralex membrane (Ralex/MF4SK/
PANI)
The membranes modified with the PANI can find an increase in
electrical conductivity and the capacity of ion-exchange mem-
branes, as well as the restriction in current density. An increase
in the restriction of current density can be related firstly to the
coated polyaniline, which increases the conductivity of surface
ion-exchange membranes and secondly the changes in surface
morphology [296]. Xie et al. [297] synthesized AEM containing
PANI as an additive and PVDF as the base to recover sulfuric acid
from waste water and concentrated it. HSO-4 ion can pass through
the molecular chain of PANI, but the hydrophobic property and
high density of the synthesized membrane inhibit proton transfer.
High-water absorption is one of the most obstacles of using
high-capacity polymeric ion-exchange membranes in capacitive
deionization due to making them unstable. To solve this problem,
Haq et al. [298] prepared an AEM using the pore-filling polymer-
ization method and used a highly porous and low-density poly-
ethylene as a supporting membrane. The cross-linking agent was
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
polychloromethyl styrene synthesized through the polymerization
of chloromethyl styrene and divinylbenzene. The newly synthe-
sized product showed improved performance to AEM and had a
higher ion-exchange capacity and lower electrical resistance.
Membrane capacitive deionization (MCDI) is known as an inno-
vative technique that could help to global water scarcity problem.
In the desalination process, MCDI removes the salt (solute) from
water (solvent) with low energy consumption compared to tradi-
tional desalination processes such as distillation. The main disad-
vantage of MCDI application is the choice of suitable and
effective ion-exchange membranes. McNair et al. [299] reported
an efficient membrane for the MCDI. Their quaternized ion-
exchange membrane with high capacity, hydrophilicity, and low
area resistance, was based on a mixture of polyethyleneimine
and PBI.
One of the clean and efficient options for future energy sources
is the AEM fuel cell. Furthermore, the stability of this type of mem-
brane limits its improvement. Kim et al. [300] enhanced AEM con-
ductivity and stability by adding unfunctionalized triptycene PES
into 1-methyl imidazolium PES to act better in fuel cells. This
improvement seems to be the result of nanophase separation and
internal free volume.
The role of polymeric additives in distillation membranes
Membrane distillation is a thermally managed separation tech-
nique. According to the mechanism used in membrane distillation,
vapors are allowed to permeate through a microporous membrane
and the liquid feed solution is retained because of the hydropho-
bicity of the membrane. It should be noted that a hydrophobic
microporous membrane is used in this technique [301].
A simple configuration of membrane distillation consists of per-
meate side and feed side with different temperatures that cause a
difference of vapor pressure over the membrane. The transport of
mass is started because of the feed liquid evaporation at the phase
border line. Then the appeared pressure causes vapor molecules to
pass through the membrane, and then condensation occurs at the
permeate side again (Fig. 11a). Four basic configurations of distilla-
tion membranes containing lower vapor pressure on the permeate
side are shown in Fig. 11b. In direct contact membrane distillation
(DCMD), permeate with lower pressure and cold temperature is in
contact with the membrane, directly. In air–gap membrane distil-
lation (AGMD) configuration, a layer of the air gap is recommended
between the permeate side in cold temperature and membrane
surface to decrease the heat loss during the conduction. Using a
cold sweep gas on the permeate side is the reason for the driving
force in sweep gas membrane distillation (SGMD). About vacuum
membrane distillation (VMD), the permeate side faces vacuum
[301]. Fig. 11b explains this method schematically.
The greatest importance and benefit of this technique are ded-
icated to separating non-volatile and salts that are dissolved in
water. This technique is used extensively to separate component
with different volatilities such as alcohols [302], volatile aromas
[303], and ammonia [304].
In membrane distillation, polymeric membranes are more com-
mon than ceramic ones. This choice is related to the lower thermal
conductivity (0.1–0.5 W.m1.k1) of polymeric membrane than
1 W.m1.k1 for ceramic membrane. PVDF, PTFE, and propylene
(PP) are the most common polymers that are suitable for MD and
PE and PES membranes were also used, recently [305].
Zheng et al. [306] used three kinds of highly hydrophobic per-
fluorinated copolymers (commercial name: Hyflon AD) in the
matrix of PVDF hollow fibers and investigated different membrane
properties such as porosity, morphology, mechanical property, liq-
uid entry pressures (LEPs), and separation performance in VMD.
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
The viscosity of the coating polymer solution affected pore size,
pore size distribution, porosity and LEPs significantly. Lower vis-
cosities of coating solutions resulted in smaller pore size, lower
porosity, limited pore size distribution, higher LEPs, and less flux
decline in VMD. Especially about LEP, using a lower viscose solu-
tion (0.46 MPa) caused LEP to be about two times higher than
the bare one (0.23 MPa). It should be mentioned that the anti-
wetting property of coated membranes was improved two times
relative to the original membranes. Consequently, the covered
composite hollow fiber membranes showed better hydrophobicity,
separation performance and mechanical property.
The role of polymeric additives in pervaporation membranes
Usually, the performance and/or the stability of polymeric PV
membranes should be improved by structural and functional mod-
ifications. Adding or grafting related functional groups to the base
polymer of the matrix is needed to improve the hydrophilicity and
hydrophobicity [307]. Among different kinds of PV membranes (or-
ganic polymeric, inorganic, and organic/inorganic blends mem-
branes), the polymeric membrane is the most cost-effective
group of the PV process. In recent years, the PV separation process
has been used extensively in organic mixture separation. Some of
the most applications of this technique were in the separation of
benzene/cyclohexane, methanol/dimethylcarbonate, methyl tert-
butyl ether (MTBE)/methanol, and ethyl tert-butyl ether (ETBE)/
ethanol mixture [307].
About the PV dehydration of organic solvents, the diffusivity of
water in the polymeric matrix of membranes and high solubility
are necessary. Consequently, the modification of polymeric mem-
branes via different approaches such as blending, grafting, copoly-
merization, and grating, can yield better membrane performance
in PV dehydration. Among different methods, polymer blending
attracts more attention due to the economical profit in addition
to physical and chemical growth [308].
Zhou et al. [309] used polypyrrole membranes doped with hex-
afluorophosphate (PF
6) and p-toluenesulfonate (CH3C6H4SO 3 ) to
study the recovery of methanol from various organic solvents
(toluene, isopropyl alcohol, MTBE and acetonitrile). Among all of
performed tests, the best methanol fluxes reached 300 g.m2.h1
(with selectivity growth from 20 to 600) which belonged to the
blend system of methanol/toluene. Amarante and Donaldson
[310] used a mixture of acetate propionate (CAP) and poly(1-
vinylpyrrolidone-co-vinyl acetate) (PVP/PVAc) for ethanol recovery
from 2-ethoxylhexanol. They investigated the effect of different
parameters including membrane composition, operational process
(e.g., temperature), and feed composition, on membrane sorption
and separation efficiency. The observed results showed that higher
ethanol fluxes were obtained in higher temperatures and higher
feed composition. However, more ethanol concentration had an
inverse proportional effect on the separation performance and
selectivity factor. They concluded that the composition of feed
and operating conditions are the most impressive parameters
and the isolate of these two could also be effective.
Devi et al. [311] used blend membranes of CS/PVP for PV dehy-
dration of tetrahydrofuran (THF). According to their report, blend-
ing CS with PVP improved water permeability and selectivity while
it decreased the membrane crystallinity. Zhu et al. [312] added PVP
to the sodium alginate (NaAlg) selective layer and increased the
hydrophilicity of polyacrylonitrile (PAN)/NaAlg composite mem-
branes. The performed modification was effective for permeation
and separation processes during caprolactam dehydration. Almwli
et al. [308] used polybutylene succinate (PBS)/PVP blend mem-
branes for the dehydration of acetone. Significant growth was
observed in different properties, such as the hydrophilicity, swel-
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al. Journal of Industrial and Engineering Chemistry 109 (2022) 100–124

Fig. 11. (a) Direct contact membrane distillation process in schematic representation, (b) Different arrangements of membrane distillation process.

ling, and tensile strength growth, of PBS/PVP blend membranes in of PVP led to higher total flux as well as better separation perfor-
comparison with the bare PBS one. Furthermore, the incorporation mance and separation index (PI) of new membranes.
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N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al.
The role of polymeric additives in contactor membranes
One of the main problems in the application of the membrane
contactor is to solve the problem of wetting the membrane during
a long time of operation. Therefore, improved hydrophobicity and
mechanical strength of the fabricated membranes are needed to
make sure the most improved transmembrane fluxes and rejection
factors for MD processes. The more attraction of polymer blends is
because of achieving the target properties of the membrane that is
totally different from the individual starting material [313]. Merin-
golo et al. [313] reported highly hydrophobic membranes, obtained
by mixing two fluorinated polymers: PVDF and its copolymer
fluoride-co hexafluoropropylene PVDF-HFP. They used the phase
separation technique in two steps, non-toxic solvents and no
chemical additive as a pore former. The useful effect of blending
was reported on the investigated properties (e.g., permeability,
surface roughness and charge, wettability and crystallinity) show-
ing a good physical interaction between two polymers despite
their immiscibility in the thermodynamical state. An et al. [314]
used PDMS microspheres as the coverage on PVDF-HFP membrane
to enhance hydrophobicity and observed improved performance.
Polymeric nanoparticle additives
Most of the water-soluble polymers used in membrane prepa-
ration, disappear during membrane fabrication and improvement,
which haven’t been considered in membrane hydrophilicity [21].
Applying polymeric nanomaterial in the range of 40–200 and an
average size of 150 nm in the polymeric matrix of membranes,
works as a bridge between bulk materials. Recently, nanocompos-
ite membranes prepared by mixing nanomaterials such as titania,
silica, silver, and carbon nanotubes (CNTs), into the casting solu-
tion have created a new base to a great improvement in the
mechanical and surface properties of membrane such as perme-
ability and antifouling [22]. By adding small and proper amounts
of nanomaterials, the porosity of membranes and, especially, the
membrane pores increased considerably in the cross-section.
Nevertheless, the large specific surface of nanomaterials has a
great tendency to agglomerate and reduce the improvement of
nanomaterial usage and even affects negatively the membrane
performance [189]. Thus, the improved performance of
nanomaterial-blended membranes, especially in industrial produc-
tion, needs to solve the agglomeration problem. Agglomeration
winded up in pure water flux reduction due to the high amounts
of NPs in the membrane matrix and the blockage of membrane
pores [22,315]. However, the agglomeration should be reduced if
the used nanomaterials have similar properties such as the poly-
mer matrix. Therefore, the functionalized polymeric NPs are being
developed for this purpose.
Fan et al. [316] used chemical oxidative polymerization to syn-
thesize PANI nanofibers, which were then dispersed in the casting
solution by intensive stirring and sonication. The result of this
modification caused improvements in permeability and antifouling
properties of membranes. Meantime, the dispersion process of
polymeric nanofibers consumed much time and energy and
resulted in a problem obtaining a homogeneous casting solution.
To overcome this problem, water-soluble polymers (such as PVP
and PEG) as an effective steric stabilizer were utilized to prevent
the precipitation of the polymeric participant, which were extre-
mely well dispersed in the polymeric solution. Coupling (either
grafting or adsorbing) of PANI nanomaterials and the steric stabi-
lizer happened after the polymerization of precipitating PANI
nanomaterials. Regarding the PANI-PVP nanocomposite, hydrogen
bonding between the N-hydrogen of the PANI and the carbonyl
group of PVP is the factor of cohesion of two parts in the PANI-
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Journal of Industrial and Engineering Chemistry 109 (2022) 100–124
PVP nanocomposite. Accordingly, one-step synthesis could be
obtained using a well-dispersed PANI-PVP nanocomposite.
Zhao et al. [317] applied a simple method to synthesize PES/PVP
polymeric NPs and used them for the modification of PES mem-
branes. They reported that the free radical polymerization tech-
nique was used to synthesize PES/PVP semi-interpenetrating
network (semi-IPN) NPs in homogeneous PES solution, N-methyl
pyrrolidone (NMP) as a solvent and N,N’-methylene bisacrylamide
(NMBAA) as a cross-linker. Semi-IPN polymeric NPs could be used
directly by blending to modify PES membranes. Using the semi-IPN
technique to synthesize polymeric NPs, makes it possible to use
them directly in the phase inversion method and fabricating
blended membranes. The incorporation of semi-IPN polymeric
NPs, obviously improved the hydrophilicity and permeability of
PES membranes.
Scofield et al. [318] applied atom transfer radical polymeriza-
tion and the ‘‘core-first” approach to synthesize soft polymeric
NPs on the basis of PEG and PEG-b-PDMS for use in membrane fab-
rication. The TFC membranes fabricated from commercially
polyamide-b-ether (Pebax2533) with PEG and PEG-b-PDMS NPs
were improved greatly in the flux and selectivity of separating
CO2 from N2 at the defined situation.
Shirke et al. [319] reported the synthesis of polymeric calcium-
alginate particles by an ‘‘egg box” structure with an emulsification
additive process to increase the performance of TFC membranes for
water vapor separation. Water vapor/N2 gas permeation data
exhibited that the presence of calcium-alginate particles in the
PA layer enlarged the water vapor permeation because of the
increased sorption site numbers and higher surface area obtained
by the particles via their huge hydrophilic functional groups.
Conclusion and perspectives
To overcome the shortcoming of membrane components, poly-
mer blending is the prominent method due to combining the effec-
tive properties of different components to make a new
composition with a specific target. In recent decades, several types
of polymer materials have been applied to fabricate membranes.
Moreover, numerous investigations have been done to obtain
improved membranes with better morphology and structures
and, consequently, increase the separation performance from the
experimental scale to module designs. These are water-soluble
polymers, and this special property increases membrane pore sur-
face and the pore-forming effect. In fact, the miscibility of polymer
blends is related to the molecular interaction between the chosen
polymers, such as hydrogen bonding and charge transfer interac-
tions. Effects of co-polymers on the thermodynamical and precip-
itation kinetic properties of the synthesized membranes were
investigated by viscosity, coagulation value, and light transmit-
tance measurements.
CRediT author statement
Nazanin Nasrollahi: Literature review, Writing- Original draft
preparation. Leila Ghalamchi: Literature review, Writing- Original
draft preparation. Vahid Vatanpour: Literature review, Supervi-
sion, Reviewing and Editing. Alireza Khataee: Literature review,
Supervision, Reviewing and Editing. Maryam Yousefpoor: Review-
ing and Editing.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
N. Nasrollahi, L. Ghalamchi, V. Vatanpour et al. Journal of Industrial and Engineering Chemistry 109 (2022) 100–124

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