High-Performance Photocatalytic Membranes For Water Purification

Journal of Environmental Management 311 (2022) 114817
Contents lists available at ScienceDirect
Journal of Environmental Management

journal homepage: www.elsevier.com/locate/jenvman
High-performance photocatalytic membranes for water purification in

relation to environmental and operational parameters
Mihaela Homocianu, Petronela Pascariu *
“Petru Poni” Institute of Macromolecular Chemistry, 41A, Grigore Ghica Voda Alley, 700487, Iasi, Romania
A R T I C L E I N F O A B S T R A C T
Keywords: Growing technologies, increasing population and environmental pollution lead to severe contamination of water
Photocatalytic membranes and require advanced water treatment technologies. These aspects lead to the need to purify water with
Dyes advanced smart materials. This paper reviews the recent advances (during the last 5 years) in photocatalytic
Antibiotics
composite membranes used for water treatment. For this purpose, the authors have reviewed the main materials
Pesticides
Water purification
used in the development of (photocatalytic membranes) PMs, environmental and operational factors affecting
Scale-up the performance of photocatalytic membranes, and the latest developments and applications of PMs in water
purifications. The composite photocatalytic membranes show good performance in the removal and degradation
of pollutants from water.
pollutants, even at low concentrations in a few hours, without forming

secondary hazardous products also having, high-efficiency, simple
1. Introduction
operation, low cost, and low energy consumption (Liu et al., 2019). The
photocatalytic process can completely degrade organic pollutants
The rapid development of nanoscience and nanotechnology has
(Chankhanittha et al., 2021; Piriyanon et al., 2021; Sansenya et al.,
provided a great number of new possibilities for water purification and
2022; Senasu et al., 2021). They are also well known for their relatively
treatment. The supply of safe drinking water is a major challenge for
low cost, low energy consumption and high efficiency. Many photo
developed countries, which has led to the growth of new technological
catalytic materials are known, including ZnO (Chankhanittha et al.,
innovations for better water management. Industrial wastewater con
2021), TiO2 (Singh et al., 2020), BiOBr (Senasu et al., 2021), WO3
tains dangerous compounds (e.g., dyes (Rose Bengal, Thymol blue,
(Piriyanon et al., 2021; Ge et al., 2021) and Bi2MoO6 (Wang et al.,
Carmine, Red 120, Indigo Red, Rhodamine B, Victoria blue, Methylene
2022), and the methods used to improve their photocatalytic activity,
Blue (Zhou et al., 2019), antibiotics (Singh et al., 2020), pesticides (Zhao
such as the addition of the noble metals, doping with transition metals
et al., 2018), pharmaceuticals (Prasad et al., 2019), and oily wastes (Li
and non-metals and forming composite photocatalysts, which has been a
et al., 2020a)), which have serious adverse effects on aquatic life and
growing research area in recent years (Gupta et al., 2020a).
humans (Chen et al., 2018). Several physical/conventional techniques
Moreover, membrane technology plays an important role in water
have been used to reduce toxic dye compounds in wastewater, including
treatment due to its interesting features, easy operation, no addition of
coagulation-flocculation, separation (Wang et al., 2020c), reverse
chemical additives (or less), cost-efficiency, no phase change, high
osmosis, precipitation, ion exchange method, ultra-filtration adsorption
productivity, easy scaling and good removal capacity. Typically, a
on activated carbon (Wang et al., 2021b), and chemical methods, such
membrane is a system consisting of a barrier that selectively allows
as photosensitive oxidation (Hao et al., 2020), adsorption (Wang et al.,
wanted materials to pass through and unwanted to retain on the mem
2019b, 2020d; Li et al., 2017b, 2019d), have been employed to reduce
brane surface (Mezher et al., 2011). In particular, photocatalytic mem
the toxic dye effluents from wastewater. The major disadvantage of
branes have unique properties, such as antimicrobial properties,
these techniques is the formation of secondary waste that cannot be
superhydrophilicity, high photocatalytic oxidation, and separation,
reprocessed and discharged as such. Instead, photocatalytic methods
which allow acting to eliminate and photocatalytic degrade the organic
consist of highly advanced oxidation processes that are used for the
pollutants, bacteria, and viruses from water. They can be used at
photodegradation of toxic compounds, they have many benefits over
ambient temperature and the target pollutants are degraded to CO2,
traditional wastewater treatment techniques, such as the removal of
* Corresponding author.
E-mail addresses: [email protected], [email protected] (P. Pascariu).
https://doi.org/10.1016/j.jenvman.2022.114817
Received 15 November 2021; Received in revised form 16 February 2022; Accepted 26 February 2022
Available online 8 March 2022
0301-4797/© 2022 Elsevier Ltd. All rights reserved.
M. Homocianu and P. Pascariu Journal of Environmental Management 311 (2022) 114817
Abbreviations PP polypropylene
PVDF polyvinylidene fluoride
AB25 acid blue PMs photocatalytic membranes
AMX amoxicillin PMMA poly(methyl methacrylate)
ANN artificial neural network PAN polyacrylonitrile
AO7 acid orange 7 PANI polyaniline
APTES 3-aminopropyltriethoxysilane PEG poly(ethylene glycol)
Ag3PO4 silver-phosphate PTFE polytetrafluoroethylene
BSA bovine serum albumin PEO polyethylene oxide
Bi2O3 bismuth oxide PES polyethersulfone
BC biochar PDMS polydimethylsiloxane
BQ benzoquinone PI polyimide
CA cellulose acetate PEI polyethyleneimine
CAP chloramphenicol PCND polycarboxylated nanodiamond
CdS cadmium sulfide PNHMA poly(N-hydroxymethyl acrylamide)
CeO2 cerium oxide PSF polysulfone
CIP ciprofloxacin PSS poly(sodium styrenesulfonate)
CuO copper oxide PVA polyvinyl alcohol
CR Congo red PVP polyvinylpyrrolidone
CV Crystal Violet PE polyethylene
CNTs carbon nanotubes PET polyethylene terephthalate
DCF diclofenac PDA polydopamine
EBT eriochrome black T PU polyurethane
E. coli Escherichia coli rGO reduced graphene oxide
EY eosin yellow RB19 reactive blue 19
FRR flux recovery rates RhB rhodamine B
GO graphene oxide ROS reactive oxygen species
GMF gemifloxacin RR11 Reactive Red 11
g-C3N4 graphite carbon nitride RR120 reactive Red 120 dye
HA humic acid Rb5 reactive Black 5
H2O2 deionized water RR195 reactive red 195
IBP ibuprofen RTB remazol turquoise blue
IC indigo carmine RO84 Reactive Orange 84
LB3R Lanasol Blue 3R SA sodium alginate
MWCNTs multiwalled carbon nanotubes SnO2 tin oxide
MB methylene blue SiO2 silicon dioxide
MO methyl orange SMX sulfamethoxazole
MCE mixed cellulose esters TiO2 titanium dioxide
MOFs metal-organic frameworks TNT titanate nanotube
NPR naproxen TrFE trifluoroethylene
NiO nickel oxide TC tetracycline
NP nonylphenol UV ultraviolet
PA polyamide ZnO zinc oxide
PA6 polyamide 6 ZrO2 zirconium dioxide
PC polycarbonates WO3 tungsten trioxide.
H2O, and N2. Another advantage of PMs is that the nanophotocatalysts photocatalytic membranes, including fabrication and characterization
need to be separated from the system. This aspect will promote the of TiO2-based photocatalytic membranes (Leong et al., 2014), the
practical use of photocatalytic membranes in water treatment (Zhang application of photocatalytic membranes for water treatment (Bas
et al., 2014). Here, photocatalysts degrade contaminants from polluted syouni et al., 2019) and H2 production (Iglesias et al., 2016), factors
wastewater generating different reactive oxygen species such as •OH, affecting membrane performance (Zheng et al., 2017). Compared to
O2− , H2O2, and 1O2, which are responsible for the mineralization of other the previously published reviews, this paper mainly reviews the
pollutants (Nasir et al., 2020). These reactive oxygen species can oxidize materials used to produce PMs, the influence of medium factors on the
organic contaminants from water. photocatalytic activity, and their connection with the performance of
The performance of a photocatalytic membrane is strongly influ PMs that are used for the degradation of various organic pollutants in
enced by the nature of the component materials, as can be seen in wastewater.
Table S1. Photocatalytic membranes prepared using different methods
exhibit varied properties in terms of membrane flux, pollutant degra 2. Photocatalytic degradation and membrane separation
dation efficiency, selectivity and antifouling performance (Li et al.,
2014). Over time, there have been many limitations in the use of pho Generally, the photocatalytic membrane processes consist of a
tocatalytic composite membranes, but also some recently found solu combination of physical separation by filtration and degradation of
tions to these problems, as can be seen in the Supporting Information. pollutants or antibacterial properties obtained from photocatalysis of a
Numerous research groups have reviewed the recent progress of given system. Thus, as is well known, photocatalytic membranes play a
2
Fig. 1. An illustration of the commonly used preparation methods of the photocatalytic membranes (PMs); (a) hydrothermal synthesis (Zhang et al., 2009),
Copyright 2009 WILEY-VCH Verlag GmbH & Co. KGaA; (b) liquid phase deposition (Pan et al., 2012), Copyright 2012 Royal Society of Chemistry; (c) in situ
reduction reaction (Liu et al., 2020), Copyright 2020 Elsevier B.V.; (d) electrospinning method (Homocianu and Pascariu, 2020), Copyright 2020 Taylor & Francis.
major role in water treatment technologies due to their simultaneous 3. Synthesis of photocatalytic membranes
separation and photocatalytic degradation. Moreover, these membranes
allow independent control of the separation and photocatalytic char A great number of photocatalytic membranes have been prepared
acteristics because they do not influence each other. using various synthesis methods, such as sol-gel (Yacou et al., 2013),
anodization (Albu et al., 2007), hydrothermal synthesis (Zhang et al.,
2009), liquid phase deposition (Pan et al., 2012), and electrospinning
(Ahmed et al., 2015). Fig. 1 shows the illustration of the commonly used
3
preparation process of the photocatalytic membranes. Recently, Liu Table 1

et al. (2020) proposed a novel strategy to prepare magnetic PVDF- Representative examples of commonly used template/membranes to incorpo
Ni–ZnO photocatalytic membranes by an in situ reduction reaction and rate catalysts for developing the further developed photocatalytic membranes.
which exhibits improved performance in water treatment. In 2020, a Template/ Characteristics Catalysts
research group (Li et al., 2020b) prepared four poly (vinylidene fluoride) Membrane
(PVDF)-based membranes (PVDF, P-CND, P–TiO2, and P-CND/TiO2) PVDF (Cui et al., - high thermal stability; TiO2 (Paredes et al., 2019;
with improved antifouling, self-cleaning and photocatalytic properties 2019) - excellent chemical and Erusappan et al., 2021);
by non-solvent-induced phase separation. A comprehensive summary of mechanical properties; 3D TiO2/ZnO (Li et al.,
- negative charge on the 2017a);
the synthesis methods, materials, and compositions used in the prepa
surface (thus limiting g-C3N4 (Kolesnyk et al.,
ration of PMs is detailed in recent review papers (Li et al., 2021; Romay biofouling). 2020);
et al., 2020, Kayvani et al., 2018). The photocatalytic membranes ob Ag–TiO2 (Salazar et al.,
tained by electrospinning can serve as substrates for the growth of 2020);
various nanoparticles and are used further for numerous applications, SnO2–TiO2 (Hong et al.,
2021);
such as the degradation of dyes (Wang et al., 2020b; Ni et al., 2019) Ag3PO4/GO/APTES (Zhang
adsorption of heavy metal ions (Habiba et al., 2017; Shariful et al., et al., 2020);
2017), water separation (Li et al., 2019e; Feizpoor and Habibi-Yangjeh, SrTiO3–Cr (Lin et al., 2019);
2018), and microbial disinfection (Wang et al., 2020b; Kim et al., PDA/RGO/Ag3PO4 (Zhang
et al., 2019b);
2018b). These membranes combine the properties of the photocatalyst
CoFe2O4 (Dorneanu et al.,
and the template membrane. 2017).
PANI (Vijayakumar - conjugated π system; Ag3PO4 (Liu et al., 2017b);
4. Types of photocatalytic membranes and Khastgir, - low cost; TiO2 (Radoičić et al., 2017);
2018) - high stability; BiPO4 (Yu et al., 2018b);
- wide absorption range silica (Vijayakumar and
Types of photocatalytic membranes depend on the placement of the under visible light; Khastgir, 2018).
photocatalyst: - hole transporting
properties.
1) the photocatalyst is solubilized/suspended in the solution, PTFE (Feng et al., - show a high resistance Mn3O4/g-C3N4 (Chen et al.,
2018) to UV; 2020a).
slurry reactors. Here, the suspended photocatalyst has a higher
- chemical stability;
surface area that leads to higher photocatalytic efficiency but ap - high heat resistance;
pears to have disadvantages associated with the recovery process. - strong hydrophobicity;
The separation, recovery, and reuse in practical applications of a - high fracture toughness.
given photocatalyst after the may require high-cost treatment and be PET ( - easy availability; TiO2 (https://scholar.google.
M-Eleftheriadou - low-cost and com/citations?user
more time, are the disadvantages of slurry reactors. The fouling
et al., 2019) renewability; =nkEwimcAAAAJ&hl
characteristics of the membrane with photocatalyst suspended in the - high mechanical =ro&oi=sraKutuzau et al.,
solution are great compared to those of membrane where the pho properties. 2019);
tocatalyst is entrapped or deposited in/on the membrane matrix CuO (Yasin et al., 2020).
PSF (Ahmadi et al., - high glass-transition N, Pd co-doped TiO2 (
(Argurio et al., 2018).
2020) temperature; Kuvarega et al., 2018)
2) the photocatalyst is entrapped or deposited (immobilized) in/ - great pH tolerance; Cu2O (Singh et al., 2019);
on the membrane. Here, no further separation of the photocatalyst - low price; mpg-C3N4/TiO2 (Yu et al.,
is required and which reduces the cost of the operation. The removal - good permeability. 2018a);
efficiency is higher in entrapped PMs because of the photooxidation WO3 (Peyravi et al., 2017);
TiO2-MWCNT (Muhulet et al.,
occurring on the outer surface and inside the membrane pores, once
2020);
the pollutants are penetrated with the carrier fluid. The loading of ZrO2–SnO2 (Zakeritabar
photocatalysts on the membrane surface increases the hydrophilici et al., 2018);
ty, which is of great importance for reducing membrane fouling and CoFe2O4 (Pascariu Dorneanu
et al., 2018a);
increasing membrane permeation flux (Zakria et al., 2021; Pascariu
NiFe2O4 (Cojocaru et al.,
et al., 2019). 2016).
PAN (Gao et al., - show a high resistance g-C3N4 (Alias et al., 2020);
2020) to UV; Cu–Fe3+ (Yi et al., 2020);
4.1. Nature of materials - high light stability; TiO2/graphene (Zhang et al.,
- excellent mechanical 2021c);
stability; ZnO (Du et al., 2021).
4.1.1. Membrane matrix materials - chemical resistance;
Supports/templates (matrix) for developing photocatalytic mem - susceptible to oxidation.
branes are usually obtained by electrospinning method that allows PES (Otitoju et al., - low cost; O-g-C3N4 (Salim et al., 2019);
2020) - excellent chemical TiO2SiO2/CoFe2O4 (
modulating the diameter and structure of the nanofibers and means the
resistance; Zangeneh et al., 2019); fGO (
large specific surface area (Gao et al., 2020). According to the literature, - high rigidity; Giwa and Hasan, 2020);
the electrospinning method gives a mixed matrix membrane consisting - thermal and biological CaCu3Ti4O12 (Otitoju et al.,
of a mixture of photocatalyst and polymer (Salazar et al., 2020). stability; 2020); ZnO/MWCNTs (
Polymers, such as polyacrylonitrile (PAN) (Shi et al., 2017; Tissera - hydrofobicity and low Zinadini et al., 2017).
UV resistance.
et al., 2018; Sun et al., 2017; Jia et al., 2019), polyvinylidene fluoride CA (Rajeswari et al., - superior transport ZnO (Hassan et al., 2017;
(PVDF) (Cui et al., 2019), polytetrafluoroethylene (PTFE) (Huang et al., 2017; Olaru et al., characteristics; Pascariu et al., 2018b; Lin
2018; Li et al., 2019b), P(VDF-TrFE) (Jia et al., 2019), PA6 (Blanco et al., 2019) - good water affinity; et al., 2019).
2019), polysulfone (PSF) (Kuvarega et al., 2018; Singh et al., 2019), - low protein adsorption;
- suitable mechanical
polyethersulfone (PES) (Giwa and Hasan, 2020), polymethyl methac
strength;
rylate (PMMA) (Hussien et al., 2020) and cellulose acetate (CA) - high hydrophilicity;
(Aboamera et al., 2018) have been largely used to produce photo (continued on next page)
catalytic mats by electrospinning. PTFE, PVDF, and PAN membranes
4
Table 1 (continued ) in water treatment (Zahid et al., 2018; Pascariu et al., 2022a). The key
Template/ Characteristics Catalysts drawbacks of TiO2 are the high recombination ratio of the electron-hole
Membrane and a broad band-gap (3.0–3.2 eV (Gomes et al., 2019)) that implies low
- excellent film forming
visible light absorption ability (only UV light (200–400 nm) that is less
property (Rajeswari than 5% of the normal sunlight). Over time, many methods, such as
et al., 2017). doping with a co-catalyst (other metal oxides ZnO (Qi et al., 2020), SiO2
PU (Rajeswari et al., - have unique mechanical ZnO (Inderyas et al., 2020); (Hu et al., 2017), NiO (Faisal et al., 2018), non-metal, and metal doping
2017) properties; GO-TiO2 (Sundaran et al.,
of TiO2, and preparation of black TiO2 by treating TiO2 with hydrogen
- increased flexibility, 2020); g-C3N4 (Svoboda et al.,
hardness, and tensile 2020). (Hu et al., 2017; Katal et al., 2018) being studied to avoid these limits.
strength; Remarkable for these materials are stability, low cost, photo activity,
- increased temperature; and nontoxicity. Titanium oxide-based membranes possess antibacterial
- resistance to extreme and antifouling properties but have a lack of established (Kim et al.,
pH.
PP (Wenten et al., - have unique mechanical ZnO (Wenten et al., 2020).
2018a). Instead, more recent studies concluded that the incorporation of
2020) properties; TiO2 into PVDF (Wang et al., 2016), PSF (Nayak et al., 2017),
- increased flexibility and PES-F-COOH (Geng et al., 2017), and polyetherimide (PEI) (Jiang et al.,
low cost. 2018) matrix conduces to obtain high-photocatalytic membranes
PMMA (Hussien - polymer with a higher CdS (Hussien et al., 2020);
because it can simultaneously affect a single surface in terms of photo
et al., 2020) transparency (that TiO2-PVDF (Errahmani et al.,
enhanced 2021). catalytic and hydrophilic properties (Carp et al., 2004). For example,
photocatalytic activity); N-doped TiO2 has enhanced UV and visible light activity (Horovitz et al.,
- low mechanical 2016; Gao et al., 2021). Numerous studies (Athanasekou et al., 2014; Xu
resistance. et al., 2016) of photocatalytic composite membranes based on syner
gistic effects between graphene oxide (GO) and TiO2 leads to enhanced
have a major advantage that consists of prolonged exposure to UV light photocatalytic activity and used for water treatment have been per
(up to 30 days of UV illumination) (Chin et al., 2006). Among these formed (Athanasekou et al., 2014; Al-Gamal et al., 2021). GO/TiO2
polymers, PVDF (Cui et al., 2019) is the most commonly used polymer incorporated in PVDF matrix also forms photocatalytic membranes with
due to its high thermal stability, excellent chemical resistance, and good potential in water treatment due to its high-performance (upon the
mechanical properties. incorporation of TiO2 and GO, the GO/TiO2-PVDF membrane displayed
For water treatment, widely used are membranes fabricated from significantly improved photodegradation efficiency toward bovine
CA, and mixed cellulose esters, MCE due to their good mechanical serum albumin - BSA (improved about 50–70%) and multifunctional
strength, especially their easy availability, superior transport charac characters, i.e. separation, photocatalytic oxidation and self-cleaning
teristics, excellent water affinity, low protein adsorption, good film- (Xu et al., 2016). The superhydrophilicity of TiO2 causes increased
forming property, and low cost (Fischer et al., 2008). Instead, these water flux under UV or sunlight conditions (Tran et al., 2020). More
natural compounds have low chemical and thermal resistance that was over, in the last few years, TiO2 - based PMs have been used by re
reduced by mixing CA with other polymers such as polystyrene (PS) searchers for the removal of pharmaceuticals from wastewater
(Rajeswari et al., 2018), polyurethane (PU) (Rajeswari et al., 2018), or treatment (Kanakaraju et al., 2018; Wang and Zhuan, 2020). Sakarkar
with nanomaterials, including graphene oxide (Aboamera et al., 2018). et al. (2020) studied the factors affecting the performance, and prop
Table 1 presents the most commonly used templates/membranes, erties of the nanocomposite photocatalytic membranes prepared by
with their advantages, as well as a list of several of catalysts with which entrapping TiO2 (1, 2, and 3 wt%) in the PVDF matrix. They investigated
they form high-performance photocatalytic membranes. the photocatalytic degradation of the remazol turquoise blue (RTB) so
lution at different pH, temperatures and findings that acidic medium and
4.1.2. Photocatalysts high temperature provide suitably membrane properties for the degra
The catalysts play a crucial role in the photocatalytic performance of dation of this dye. After 2 wt% of TiO2 in photocatalytic membranes, the
a given photocatalytic membrane. When choosing a photocatalyst agglomeration of the photocatalyst TiO2 became dominant.
essential are the bandgap energy, chemical and photophysical stability By the synergy of the most used photocatalyst TiO2 with another
(Fatima et al., 2019), specific surface area, particle size distribution, metal oxide, (like ZnO (Upadhyay et al., 2019; Gupta et al., 2020b);
crystallographic structure and composition, non-toxic nature, ability to CeO2 (Lara-López et al., 2017), ZrO2 (Abdi et al., 2019), Bi2O3 (Ratova
its recovery and reuse, and low cost (see details in Section 4.1.). A et al., 2019), Ag3PO4 (Wang et al., 2019a), and WO3 (Arce-Sarria et al.,
comprehensive literature review (Romay et al., 2020) about synthesis 2018) and optimizing operating parameters, numerous research groups
methods, materials, compositions, of numerous photocatalysts (Liao have developed new composite photocatalytic membranes that exhibit
et al., 2018) has recently been published (Zakria et al., 2021). A pho enhancing photocatalytic degradation of pollutants from water.
tocatalyst having a lower band gap requires less photon energy. This ZnO composite membranes: Zinc oxide nanoparticles have similar
review focuses on the role of these materials in the final PMs and their photocatalytic activity as TiO2 nanoparticles, but they are more stable
influences on the performances of PMs in water treatment. The specific and less expensive. ZnO nanoparticles are capable of absorbing light
properties of 2D nanomaterials including nano-sizes, chemical structure, with a wavelength between 350 and 470 nm, while TiO2 is capable of
and morphologies of 2D nanostructured materials suggest that these absorbing light only between 400 and 420 nm. ZnO photocatalyst
materials be used in photocatalytic processes (Homocianu and Pascariu, incorporated in the membrane photocatalytic reactor demonstrated
2020; Pascariu and Homocianu, 2019). greater effectiveness than TiO2 in some cases (Hairom et al., 2014).
The role of metal oxide nanoparticles (photocatalysts) in the mem Outstanding performance has been achieved for PAN membranes with
brane matrix consists of (a) changes in the morphology of membrane in the addition of GO/ZnO for methylene blue (MB) and indigo carmine
synthesis; (b) the improvement of membrane hydrophilicity due to the (IC) dye degradation under visible light irradiation (lamp power 150 W)
photocatalyst polarity. (Abdel-Mottaleb et al., 2019). The authors reported the efficiency of up
TiO2 composite membranes: Titanium dioxide (TiO2) appeared to to 96% for MB after 70 min and 98% for IC after 27 min at an initial
be the most widely used photocatalyst for the fabrication of photo concentration of 10 mg/L.
catalytic membranes as a result of their photocatalytic, antifouling Other important photocatalysts with broad light absorption and
ability, and hydrophilic nature for the degradation of organic pollutants adjustable bandgap, such as Cu2O (Singh et al., 2019), WO3 (Peyravi
et al., 2017), ZrO2 (Ji et al., 2017), ZnO/CuO (Alzahrani, 2018), and
5
g-C3N4 (Zhang et al., 2021b; Ong et al., 2016; Mamba and Mishra, 2016)
are for developing PMs used for the decomposition of organic pollut
ants. Zhang et al. (2021b) exhibited that g-C3N4 is a visible-light-driven
photocatalyst with tailorable structures and good stability, which are
excellent for membrane applications. In this recent review paper, it is
shown that the photocatalyst g-C3N4 incorporated into different poly
meric membranes have been used in diverse applications for various
wastewater treatments. This photocatalyst is favored due to its bandgap
for visible light reactions. Due to the two-dimensional (2D) monolayer
structure, excellent adsorption property, antibacterial and photo
catalytic capabilities, highly oxide-active character, excellent electrical
conductivity, high surface area, charge mobility, catalytic performance,
durability, the graphene oxide (GO), is other important nanomaterials
commonly used for water purification (Sundaran et al., 2019; Li et al.,
2019b).
In many studies, to increase the pore size and the number of pores of
target membranes, some researchers incorporate other additives or Fig. 2. A summary of the major factors that affect the photocatalytic degra
fillers to the polymer, such as polyvinylpyrrolidone (PVP) (Zangeneh dation of pollutant materials from water.
et al., 2019), polyethylene glycol (PEG), and different inorganic salts
(Song et al., 2014). the rate of the photoreactions increases linearly with the rise in the light
intensity because the electron-hole formation is predominant and the
5. Factors affecting the photocatalytic degradation of pollutant electron-hole recombination is negligible. Instead, at the intermediate
materials from water light intensity, the photoreactions depend on the square root of the light
intensity as the separation and recombination of electron pairs compete
Although, the photocatalysis process occurs under mild operational at this point. Moreover, at high light intensities, the reaction rate is in
conditions, including ambient temperature and pressure, very few dependent of this.
auxiliary additives, and short reaction times (Molinari et al., 2010), the Temperature: Usually, photocatalytic reactions occur at room tem
photodegradation of organic compounds is highly dependent on perature. Many studies have suggested performing the photocatalytic
numerous parameters, such as the concentration of substrate, type, and process at a temperature between 20 and 80 ◦ C. For example, Mozia
amount of photocatalyst, the surface area of photocatalyst, the tem (2010) analyzed and found that the optimum temperature range where
perature of the medium, the pH of the solution, light intensity and the photodecomposition rate increases are between 20 and 60 ◦ C. At
irradiation time, doping of metal ions and nonmetal of photocatalyst and temperatures higher than 80 ◦ C are unfavorable for photocatalytic
substrate. processes, due to the promotion of electron/hole recombination and the
Among these parameters, the photocatalytic degradation and effi exothermic adsorption of the contaminant has a disadvantage, instead of
ciency of the photocatalytic membranes are highly dependent on some in the extremely low temperatures (below 0 ◦ C) as a result of desorption
operational parameters, as discussed below. of compounds from the photocatalyst surface the photocatalytic process
Structure and morphology of membranes: The structure and becomes a limited step (Zheng et al., 2017), here increases reactant
morphology of membranes have significant impacts on their charac absorption.
teristics and performances. pH: This parameter plays an important role because it influences the
Photocatalyst loading: The catalyst load depends on each system and catalysts aggregation and the surface charge of the catalyst and thus
is essential for degradation, but most often with a range between 0.04 controls the removal efficiency of the pollutants (Sakarkar et al., 2020).
and 5.0 g/L. Usually, as the catalyst loading increases the surface area of Determining the optimal pH of the solution will enhance the flow and
catalyst available for degradation and adsorption is increased and the reduce membrane fouling.
rate of degradation of dyes and pollutants will also increase (Lei et al., Dissolved oxygen: It plays an important role in the photocatalytic
2018). The more photocatalyst, the more electron-hole pairs are pro system for water treatment. The presence of dissolved oxygen in the
duced in the system, which generates more hydroxyl radicals. Initially, system inhibits electron-hole recombination in the photocatalyst,
the rate of the photoreactions is proportional to the content of the increasing mineralization, radical formation and catalyst stability.
photocatalyst from the solution, but also at high photocatalyst concen Ions: The presence of ions influence positive or negative the rate of
tration, the increased particle-particle interactions lead to surface area the photocatalytic process. The inorganic ions (Cl− , NO3− , SO42− , CO32−
loss by agglomeration. Alternatively, a higher amount of catalyst may and HCO3− ) from water decreases photocatalytic activity by scavenging
also decrease light intensity, slow reaction kinetics, low efficiency, and holes (hCB) and hydroxyl radical (•OH) (Borthakur and Das, 2018).
catalyst fouling (by blocking the sites or pores) (Molinari et al., 2010). In addition to the above-mentioned parameters, which influence the
The optimum loading of the photocatalyst in the photocatalytic mem kinetics of heterogeneous photocatalysis, a faster reaction is influenced
brane depends on the structure and morphology of the membrane, light by the following process parameters, such as dissolved oxygen, flow
intensity, and the flow rate of water. rate, a type of pollutant, concentration of the pollutant, catalyst size
Light wavelength and intensity: When setting the process parame (interfacial surface area), and irradiation time (Sundar and Kanmani,
ters, the bandgap energy to activate the photocatalyst must be correlated 2020). When the pollutant concentration is high, the surface of the
with the wavelength of the light source. Light intensity is responsible for photocatalyst can be saturated, reducing the photodegradation effi
the photocatalytic reaction rate (Loeb et al., 2019). High efficiency in ciency of the system and irradiation. For this reason, it is tried con
the solar spectrum region results in increased photocatalytic efficiency. ducting catalytic tests under water-relevant experimental conditions,
For a long time, the most widely used light sources were low-efficiency and at a concentration of contaminants that is similar to that found in
UV lamps with UV-A (λmax = 355–365 nm) and UV-C (λmax = 254 nm) wastewater. The agglomerations of pollutants increase the turbidity
because UV light sources allow for higher photonic flux. Newer many solution, which will reduce the light transmission through the solution
research groups the use of solar and high-efficiency light-emitting di and therefore decrease photocatalysts activity.
odes (LEDs) as durable irradiation sources (Jallouli et al., 2018; Gao Furthermore, the numerous parameters described above have moti
et al., 2017; Ye et al., 2018; Biancullo et al., 2019). At low light intensity, vated researchers to adapt and develop, recently, some studies on the
6
Table 2 Table 2 (continued )

Photocatalytic membranes for organic dyes degradation. PMs Experimental conditions Pollutants Refs.
PMs Experimental conditions Pollutants Refs. (initial concentration;
(initial concentration; removal efficiency (%);
removal efficiency (%); light source; exposure
light source; exposure time)
time)
98%; 40 min; UV light; Rajeswari et al.
PAN/GO-ZnO 10 mg/L; 98%; visible MB Abdel-Mottaleb neutral pH (2017)
light; 70 min et al. (2019) nylon/Bi2O3 visible light 68% RhB; RhB Gadhi et al.
PAN/ 20 mg/L; 98.5%; 275 W; MB Sun et al. (2017) 180 min (2021)
α-Fe2O3@rGO 120 min
PAN/g-C3N4 97.3%; visible light; 300 MB Alias et al. (2020)
min use of artificial neural network (ANN) methods (Mousavi et al., 2020; de
3+
PAN/Cu–Fe 0.20 g; >99.99%; 365 RB19, RR195, Yi et al. (2020) Luna et al., 2020; Talwar et al., 2019; Ayodele et al., 2020) applied for
nm, UV lamp, 60 min AO7
the design, modelling, and optimization of operational parameters of the
PVDF/GO/ZnO 10 mg/L; 86.8%; Xe MB Zhang et al.
lamp (300 W); 100 min (2019a) photocatalytic process used in the degradation of organic pollutants.
PVDF/ 10 mg/L; 91%; UV light; RhB Hong et al. The ANN technique represents a good tool for determining the optimal
TiO2–SnO2 270 min (2021) process conditions and optimizing those (Ayodele et al., 2020).
PVDF/ 80%; visible light; 30 MB Li et al. (2017a) In summary, Fig. 2 shows the major factors that affect the photo
TiO2–ZnO min
PVDF/3D TiO2/ 2 g/L TiO2; 91.42%; UV LB3R Luo et al. (2020)
catalytic degradation of pollutant/contaminant materials from water.
PSS light irradiation
PVDF/3D CNTs/ 89.31% visible light RhB Shi et al. (2020) 6. Water purification
MCU-C3N4/ irradiation
GO
Over time, separation, chemical reaction, and biodegradation are
PVDF/TNT catalyst loadings Rb5, PR Subramaniam
(0–1.0%); UV light; et al. (2018) typical water purification methods (Qayum et al., 2019). Chemical re
78.1%; 240 min action and biodegradation suggested a greater risk of secondary
PVDF-ZnO/ 99.62%; UV light; 300 RR120 Rosman et al. contamination. Instead, separation techniques (i.e., centrifugal (Klasson
Ag2CO3/Ag2O min (2019)
et al., 2005), filtration (Shi et al., 2013), absorption (Zhang and Seeger,
PSF/N–TiO2 92%; visible light EY Kuvarega et al.
irradiation (2018)
2011) exhibit high energy consumption, low efficiency, secondary
PSS/TiO2 30 mg/L;91.42%, after 5 LB3R Luo et al. (2020) pollution and lies in the unchanged molecule or chemical bond during
cycles; UV light water purification process (Wang et al., 2015). Photocatalysis using
PVDF/N–TiO2 100%; UV light (30 W); Rb5 Kamaludin et al. solar energy for clean water has been extensively studied and recognized
360 min (2019)
as one of the most sustainable methods. When photodegradation tests
PET/TiO2 35%; UV-A/Vis (36 W); Carbendazim Marcelino et al.
420 min (2019) were performed in real waters, several studies reported a decrease in
PES/ 74.83%; UV-C (360 W); RhB Otitoju et al. photocatalysis efficiency compared to the analysis performed in pure
CaCu3Ti4O12 40 min (2020) waters (Ye et al., 2018; Kanakaraju et al., 2015). TiO2-based PMs are
PANI-TiO2/rGO 0.806 mmol h− 1 g− 1; RhB Ma et al. (2020)
extensively studied for the removal of toxic organic and inorganic con
90.5%
PA6/TiO2 3 mg/L; 80%; UV (365 Remazol Blanco et al.
taminants from water, as can be seen in a recent literature review (Riaz
nm); 240 min Black B (2019) and Park, 2020; Khasawneh and Palaniandy, 2021; Chen et al., 2020b).
PMMA/TiO2 10 mg/L MO; UV MO Li et al. (2017d) Many persistent toxic substances from water sources include dyes, pes
illumination; 50 min ticides and pharmaceuticals.
PMMA/CdS 10 mg/L RhB; 18 W; RhB Hussien et al.
420 nm (2020)
PMMA/TiO2 2 mg/L; ~100%; UV MB Vild et al. (2016) 6.1. Photocatalytic degradation of dyes from water
illumination; 120 min
PVP/TiO2–Cu 0.04 g; 15 W daylight MB Zhang and Liu Organic dyes resulting from textile, paper, leather, pharmaceuticals,
lamp (2021a)
PVP/TiO2–Ag 10 mg/L; visible light; 5 MB, CR, Pascariu et al.
and food processing are one of the most important classes of contami
h (99% MB degradation) amaranth (2021a) nants from wastewater that adversely influence human and aquatic life.
PCND/TiO2 100 mg L− 1; ~82%; Xe MO Li et al. (2020b) These compounds usually have an aromatic molecular structure that is
lamp (300 W); 90 min difficult to remove/degrade. The use of photocatalytic membranes to
Chitosan/ZnO 25–100 microM; CV Abarna et al.
remove and degrade the dyes from water has received a great deal of
~100%; Tungsten lamp; (2019)
300 min interest in recent years (Chen et al., 2020; Donkadokula et al., 2020).
PP/ZnO 25 mg/L, 59%; UV MB Prasert et al. Among them, the nanofibers membranes have been used mostly for the
illumination; 300 min; (2020) degradation of dyes, such as CR, MB, MO, RB5, and RhB in concentra
100 g/L dosage tions from 10 to 20 mg/L (Pasini et al., 2020), under UV light irradia
PANI/ZnO 30 mg/L; 89%; AB25 Gilja et al. (2018)
simulated solar
tion, in 60–240 min interval time.
irradiation; 60 min; 1 g/ In Table 2, we have listed several representative papers from recent
L dosage years. In 2020, Luo et al. (2020) developed a PSS/TiO2 hierarchical
PI/Ag/ZnO/Ag 2 mg/L; 98%; UV light MB Lu et al. (2019) layer-by-layer photocatalytic membrane for strong degradation of
source; 120 min
Lanasol Blue 3R (LB3R, 91.42%, after 5 cycles, see Fig. 3a). The results
PSF/Fe-doped 10 mg L− 1, 90%; Xenon BPA Wang et al.
TiO2 lamp; 180 min (2017b) showed that this layer-by-layer self-assembly membrane has a strong
PNHMA/ 78% MO Zou et al. (2019) catalytic activity. Moreover, the authors found that after protein fouling
Ag–AgCl with BSA and 8 h of UV irradiation, the recovery rate was improved at
PVA/Pd 40 mg/L MB; up to 99%; MB, CR Yin et al. (2020) 95.41%. Moreover, this membrane has a self-cleaning ability, which is
decorated PD- 30 min
SiO2
assisted by photocatalysis.
CA-PU/ZnO RR11, RO84 A photoresponsive nanosheet graphitic carbon nitride (g-C3N4)
embedded polyacrylonitrile (PAN) nanofibres (Alias et al., 2020) was
found to show good photocatalytic activity (97.3% degradation of MB
7
Fig. 3. Degradation of various dyes using

PMs, under light irradiation, for different
times: (a) MB (Liu et al., 2020) Copyright
2020 Elsevier B.V.; (b) RB19 (Yi et al., 2020)
Copyright 2019 Elsevier Inc.; (c) RhB (Hong
et al., 2021) Copyright 2021 Royal Society of
Chemistry; (d) The degradation performance
of PSS/TiO2 towards Lasanol Blue 3R (LB),
with variations in layer-by-layer degree (1,3,
5,7 and 9) (Luo et al., 2020) Copyright 2019
Elsevier B.V.; (e) Recycling of MB by 1.0 M
TiO2-coated YSZ/silica nanofiber under
UV-light irradiation, with six times of
cycling uses (Huh et al., 2020) Copyright
2020 Springer Nature; (f) Influence of
different scavengers (IPA, EDTA-2Na and
BQ) during the photocatalytic degradation of
RhB in the presence of BiOBr@TiO2-NFM
under visible-light irradiation (Cai et al.,
2018) Copyright 2018 Royal Society of
Chemistry. (For interpretation of the refer
ences to colour in this figure legend, the
reader is referred to the Web version of this
article.)
under visible light irradiation) for wastewater treatment. This study alginate (SA), bovine serum albumin (BSA) and yeast solutions,
reveals that PAN nanofibers effectively adsorb MB species inside the respectively, which are comparable or much better than most of the
nanofibers. Strong relationships between the concentration and degra literature data.
dation of MB open a way for the use of this system in the treatment On the same topic, Pascariu et al. (2021b) prepared membranes
application of wastewater containing MB. Another literature study re consisting of La3+ doped ZnO nanofibers electrospun on PVDF sup
ported the magnetic field-assisted fabrication of the PVDF/Ni co-doped ports. The photocatalytic efficiency of PVDF/ZnO:Ln (Sm, La, Er) sys
ZnO membranes (Liu et al., 2020) and having magnetic and photo tems were evaluated in the photocatalytic degradation of MB and RhB,
catalytic properties and higher antifouling performance than that of under visible light irradiation of a polluted solution. The obtained re
bare PVDF membranes. These membranes can degrade 50% MB within sults show that these membranes present a good photodegradation
105 min at the same time having ultrahigh flux recovery rates (FRR) to (96.33% for MB and 93.36% for RhB) using the PVDF membrane con
100%, 100%, 83% and 83% for filtration of humic acid (HA), sodium taining 37% ZnO:La under visible light for 360 min. These results
Table 3
Summary of recent photocatalytic membranes used to remove antibiotics from wastewater.
Antibiotic/concentration Degradation efficiency PMs Catalyst/ Light source Ref.
concentration
CIP; 10 mg/L 99.0% CIP, 50 min PANI/Bi4O5Br2 1.33 g, BiBr3 λ > 420 nm Xu et al. (2019)
TC; 20 mg/L 85.7% TC, 240 min
CIP; 10 mg/L 99.5% CIP, PVP/La3+:TiO2 0.1% La3+ visible light Pascariu et al. (2022b)
300 min
TC; 100 μg L− 1 92%; 36 h PVDF/ZnIn2S4 0.45 g, ZnIn2S4 visible light Gao et al. (2018)
TC; 20 μg L− 1 90.8%; 60 min CNCT/g- g-C3N4@Co–TiO2 300 W, λ > 420 nm Song et al. (2020)
C3N4@Co–TiO2
TC; 20 mL 75%; 120 min PVDF/Au–TiO2 0.5 g, Au–TiO2 Xe lamp (300 W) Yan et al. (2021)
TC; 10 mg/L 87.4%; 3 h PVDF/CuO@CuS 10 mg, CuO@CuS visible light Liu et al. (2021)
norfloxacin 80.7%; 300 min PVDF-HFP/Ag–TiO2 – visible light Salazar et al. (2020)
IBP 86%; 60 min PSF/Cu2O – visible light Singh et al. (2019)
GMF 92.7% Zn–Co-LDH@BC – UV light Gholami et al. (2020)
SMX 69%; 30h mpg-C3N4/TiO2/ – – Yu et al. (2018a)
PSF
AMX 90%; 120 min; pH 5, H2O2 TiO2-GO/Fe3O4 27 wt% -TiO2- UV light Li et al. (2019c)
Fe3O4
CAP 61.59%; 120 min PSF/4 wt % TiO2- 4 wt % TiO2-HAP UV illumination Singh et al. (2020)
HAP
Mixture of: Lincomycin, Moxifloxacin, almost completely degraded PET/TiO2 1 mg/L; TiO2 under simulated solar M-Eleftheriadou et al.
Isoniazid, Metronidazole and Norfloxacin upon 360 min irradiation irradiation (2019)
8
evidenced that the introduction of 37% ZnO:La on PVDF permits The presence of Ag nanoparticles induces light absorption, large surface
obtaining an enhanced photodegradation of organic pollutants, such MB area, and effective charge separation, and thus this means that prepared
and RhB. Moreover, remarkable photocatalytic stability was observed Ag@ZnO/TiO2 membranes exhibited greater photocatalytic degrada
after ten cycles (98%) of reuse. tion efficiency of 91.6% toward tetracycline hydrochloride within 1 h,
https://www.sciencedirect.com/science/article/pii/S1385894 and show prominent antibacterial activity (after 1 h of simulated solar
716315339Rajeswari et al. (2017) studied the degradation of Reactive light exposure). According to www.sciencedirect.com/science/artic
Red 11 and Reactive Orange 84 dyes from water by ZnO blended cel le/abs/pii/S0376738820313247Zhang et al. (2021d) Ti3+-TiO2 photo
lulose acetate-polyurethane (CA-PU) membrane compared to pure catalytic membranes were prepared by a combination of hydrothermal
CA-PU membranes under different experimental conditions, such as reaction and low-temperature vacuum-activation methods and showed
irradiation time, pH and different initial concentration conditions. The enhanced photodegradation of tetracycline and anti-fouling ability
CA-PU/ZnO membrane exhibits improved photocatalytic activities over under visible light irradiation. The improved performance was due to
the CA-PU membrane at 40 min UV-light irradiation, with an optimum the high concentration stable Ti3+ centres, which are more active spe
pH of 7. cies. These photocatalytic membranes displayed 95.9% and 81.2% ef
In this section and Table 2, we have highlighted significant progress ficiency in TC degradation, upon 100 min visible light irradiation and
in the efficiency of photocatalytic membranes used for the degradation antifouling ability, for practical wastewater treatment.
of organic dyes, operating under different experimental conditions. More recently, a novel Z-scheme 2D/3D g-C3N4/BiOI-based β-phase
Based on the data summarized in Table 2, the best results were obtained PVDF photocatalytic membranes (Cui et al., 2021) have an exceptional
for PMs containing photocatalyst TiO2 (commercially available, repro photocatalytic degradation efficiency for tetracycline (94.6%) compared
ducible and stable) incorporated in numerous membrane templates, with CN/BI heterojunction power (84.0%) and two other control
such as PSF, PCND, PVP, PMMA, PA6, PANI/rGO, PET, PVDF, and PSS. membrane matrices (CN/BI/PAN and CN/BI/CA PMs) within 120 min.
Recently, a multifunctional nanocomposite membrane Ag–TiO2/
6.2. Photocatalytic degradation of pharmaceuticals from water PVDF-HFP (Salazar et al., 2020) was used to degrade norfloxacin under
ultraviolet (UV) and visible radiation. These nanocomposite membranes
Antibiotics, antiinflammatory, and antimicrobials are well-known with different concentrations of TiO2 and Ag–TiO2 were found to be
pharmaceutical products from wastewater. Antibiotic residues are photoactive to UV and visible light. The nanocomposites with Ag–TiO2
considered a major type of emergent pollutant from water. Based on show the highest degradation efficiencies: 64.2% under UV and 80.7%
extensive literature data (Antoniadou et al., 2021) different types of under the visible radiation, for 90 and 300 min, respectively. Also,
antibiotics, (including tetracycline, IBP, ciprofloxacin, sulfamethoxa antimicrobial tests were performed against two bacterial species (gram
zole, and erythromycin), at high concentrations, in all water sources + and gram -).
were found. Actually, more attention has been paid to A photocatalytic system constructed from the NiO/m-TiO2 nano
visible-light-driven photocatalysis for degrading antibiotics, as can be composites at different NiO contents (Faisal et al., 2018) showed the
seen in Table 3. complete degradation of gemifloxacin mesylate (20 mg/L) after 180 min
Researchers have reported complete removal of some commonly of visible light illumination. It was observed that it exhibited excellent
used pharmaceuticals such as ibuprofen, naproxen, and cetirizine under photocatalytic performance compared with either pure NiO or m-TiO2
UV light irradiation (Mohamed et al., 2018), within 120, 40, and 25 min, photocatalysts under visible light illumination.
while the same antibiotics under the action of the visible light irradia Ibuprofen (IBP) is a pharmaceutical from the class of nonsteroidal
tion (Uheida et al., 2019) the complete (up 99%) degradation was anti-inflammatory drugs typically used for treating fever and inflam
achieved within 200, 50, and 90 min, using surface-modified TiO2 mation, with low toxicity, higher efficiency, fruitful results that make its
nanoparticles immobilized on polyacrylonitrile/multiwall carbon excess usage and become an emerging organic micropollutant. Recent
nano-tubes composite nanofibers. studies (Singh et al., 2019) have demonstrated that Cu2O photocatalyst
In the visible light photo-degradation of antibiotics, tetracycline (TC) modified PSF matrix membranes prepared using the phase inversion
is one of the most studied antibiotics. For example, Oseghe and Ofomaja technique were successfully used to remove IBP under visible light. The
(2018) using C-doped TiO2 (0.3 g/L) with visible-LED light illumination Cu2O photocatalyst exhibits a positive effect on membrane hydrophi
(2 h) removed 70% of TC (5.0 mg/L). Recently, Wu et al. (2021) found licity and antifouling nature of the membrane, by improved flux from
that Black TiO2 exhibits much higher TC (66.2%) removal efficiency 34.24 L m− 2 h− 1–179.54 L m− 2 h− 1 and water contact angle decreased
than white TiO2 (43.4%). Also, the authors established that TC can be from 71.5◦ to 45.3◦ values. The highest amount of the Cu2O photocat
mineralized by black TiO2 under visible light irradiation, but not by alyst modified PSF membranes showed efficient removal of IBP under
white TiO2. Instead, in 2021, Luo et al. (2021) using a PVDF photo simulated light and acidic conditions, with a removal rate of 32.63 ×
catalytic membrane based on NCQDs/BiOBr/TiO2 heterojunction suc 10− 3 min− 1 and an efficiency of 86%. Simsek (2017) was reported that
ceeded to reach a TC degradation rate of 77% within 120 min, under IBP was successfully degraded in the presence of boron (B)-doped TiO2
visible light irradiation. Also, Zong et al. (2021) fabricate a compared to pure TiO2 (removal rates of 85% and 25% for B-doped TiO2
photo-response and superwettable NiAlFe LDH/PDA/PVDF membrane and pure TiO2, respectively), due to the enhanced crystallinity and
that showed high oil-in-water emulsion separation performance (>99%) electronic properties of TiO2. The effects of g-C3N4/TiO2/Fe3O4@SiO2
and can effectively degrade tetracycline, within 20 min under UV light heterostructured nanophotocatalyst (Kumar et al., 2018) on the effi
irradiation. ciency of enhanced photocatalytic removal of ibuprofen from real
Song et al. (2020b) reported a highly flexible, core-shell hetero sewage effluent under visible light were investigated. A photocatalytic
structured, and visible-light-driven membrane assembled from performance (97% IBP removal at 15 min of visible light irradiation at
g-C3N4@Co–TiO2 and PVP, matrix, which served as excellent photo pH 7), from real sewage effluent, was recorded and more than 87%
catalytic membranes. These membranes have good reversibility and removal efficiency was maintained even after 3 consecutive recycles.
recyclability. Advantages of three-dimensional porous networks These aspects indicate the great potential of this system for practical
enhanced visible-light response induced a prominent photodegradation environmental applications.
efficiency of 90.8% toward tetracycline hydrochloride, after 60 min Another nonsteroidal anti-inflammatory drug, namely, naproxen
visible light irradiation and displayed excellent antibacterial perfor (NPR) exist in excess in surface water, groundwater, wastewater,
mance (E. Coli inactivation after 90 min of visible light exposure). In a seawater and even in drinking water, at concentrations ranging from
similar study by Song et al. (2020a) a ternary Ag@ZnO/TiO2 fibrous 10− 1–105 ng L− 1 (Lancheros et al., 2019) and was studied under
membrane was used to photodegradation of tetracycline hydrochloride. UV–visible irradiation. Photocatalysis is one of many methods (e.g.
9
Fig. 4. (a) Photocatalytic degradation of

different antibiotics in the presence of PET-
10% wt TiO2 composite (50 mg) in waste
water (C0 (drug) = 1 mg/L, I = 500 W m2)
(M-Eleftheriadou et al., 2019) Copyright
2019 Elsevier Ltd.; (b) Removal efficiency of
amoxicillin (AMX) in different reaction sys
tems (Li et al., 2019a) Copyright 2019
Elsevier B.V.; (c) Effects of different light
sources on the degradation of the AMX (Li
et al., 2019a) Copyright 2019 Elsevier B.V.;
(d) Effects of pH on the degradation of the
AMX (Li et al., 2019a) Copyright 2019
Elsevier B.V.
adsorption, sono-assisted processes, ozonation, photo-Fenton and 6.3. Photocatalytic degradation of pesticides from water
advanced oxidation processes) used to remove naproxen. For example,
Torki and Faghihian (2018) photodegrade NPR using Fe3O4@PPY(pol Pesticides are the second most dangerous compound water
ypyrrole)-NiS, at pH = 7, under visible light irradiation and obtained an contaminant among various organic pollutants and represent a signifi
efficiency of 87%, within 30 min. Instead, under similar conditions (pH cant human and environmental risk (Khan and Pathak, 2020). One of the
= 7, visible light irradiation-lamp 500 W), using the titanate nano persistent pesticides from water is Endosulfan (Arisekar et al., 2019).
material, a research group (Fan et al., 2019) failed to degrade 100% Many metal-organic frameworks (Cu-MOF, Zr-MOF, Zn-MOF, and
NPR, upon 180 min of irradiation. Al-MOF) having a porous structure and highly photocatalytic activity
Great interest in the potential practical application shows the were used over time to remove several pesticides (Liu et al., 2017a;
degradation of a mixture of antibiotics from wastewater. M-Elefther Wang et al. 2020a; Ahamad et al., 2020).
iadou et al. (2019) tested the photocatalytic activity of PET/TiO2 (10%, In recent years, regarding photo-pesticide degradation, notably,
30%, and 47% TiO2) systems on the degradation of the antibiotic mix Ahamad et al. (2020) reported MoS2/ZnS embedded in N/S doped car
tures (Isoniazid, Metronizadole, Sulfadiazine, Sulfamethoxazole, bon for photocatalytic degradation of pesticides. The authors find that
Trimethoprim, Norfloxacin, Moxifloxacin and Lincomycin, see Fig. 4) in approximately 85% degradation of dicofol was achieved by the nano
the water and wastewater matrix. PET-10% wt TiO2 exhibited high composite photocatalyst and the catalytic activities remain around
performance even after 5 cycles of reuse and at higher TiO2 loading, the 77.2% after investigating the stability and reusability via five cycles.
reusability of the photocatalysts decreased. The results showed that Also, Abdelhameed et al. (2021) employed a Cu-MOF@cellulose acetate
PET-10%-TiO2 was efficient in degrading the antibiotic mixture in water membrane for the selective removal of dimethoate pesticides from
as follows: Lincomycin, Moxifloxacin, Isoniazid, Metronidazole and wastewater. These materials also showed high adsorption capacity
Norfloxacin were almost completely degraded within the first 2 h of (282.3–321.9 mg/g) and good recyclability (the adsorption efficiency of
irradiation, while trimethoprim, sulfadiazine and sulfamethoxazole the membrane was diminished by 22.5%, after 5 reusing cycles). Zhao
required a more prolonged time for complete disappearance (90, 93 and et al. (2020) prepared g-C3N4/Ag NPs intercalated GO composite
98% degradation respectively after 6 h of treatment). membrane, which under visible-light irradiation can photocatalytic
Many photocatalytic membranes have been used for the photo degradation of paraoxon-ethyl pesticide. The results showed that 92.8%
catalytic degradation of the most consumed antibiotics and anti- of paraoxon-ethyl could be degraded after 150 min visible-light irradi
inflammatory drugs (ciprofloxacin, norfloxacin, tetracyclines, nap ation. Afterwards, Luna-Sanguino et al. (2020) produce TiO2-rGO
roxen, and ibuprofen) under visible light irradiation. Note that it is nanocomposite materials for solar photocatalytic degradation of pesti
difficult to determine the most efficient PMs used in the photo cides at the pilot plant scale. It can be observed that TiO2 is uniformly
degradation of pharmaceuticals from wastewater, as the reported results distributed on rGO surfaces forming a network structure. The photo
were obtained under different conditions and are mainly limited by the catalytic capacity of TiO2-rGO was investigated for the removal of pes
scale-up of studies from laboratory to industrial scale, the most efficient ticides, including methomyl, pyrimethanil, isoproturon and alachlor, by
reuse of the system and the removal of photocatalysts from wastewater using H2O2 or O2 as the oxidants, under solar irradiation at pilot-plant
after treatment. scale. The use of H2O2 as an oxidant agent demonstrated an enhance
ment of pesticides removal, compared to using O2. Complete removal of
pesticides was achieved at very short times (<25 min).
In a recent review, a research group (Arisekar et al., 2019) concludes
Table 4
Some recent PMs used for the degradation of pesticides under light irradiation.
PMs Pesticide Target Light source/degradation rate Ref.
TiO2-rGO methomyl complete degradation; 25 min irradiation Luna-Sanguino et al. (2020)

TiO2/SiC foams paraquat UV-C (254 nm); 91%; 3h Marien et al. (2019)
PVDF/PDA- roxarsone ~100%; 3h; visible light Zhou et al. (2020)
BiOCl0.875Br0.125
PES/Co/TiO2 2,4-dichlorophenol (2,4- 2,4-DCP (40 mg/L); catalyst weight (50 mg); visible light irradiation; 53%; 120 min. Hoseini et al. (2017)
DCP)
10
Table 5
Recently developed methods used for the enhancement of photocatalytic efficiency for the degradation of different pollutants from water.
PMs/pollutants Photocatalytic response Methods Ref.
a) b)
PVA/TiO2 MB 56% 73% - plasma treatment. Montallana et al.

(2020)
PVP/rGO@TiO2 MO 52.4 mg removed 112.4 mg removed - enhancement of photocatalytic degradation due to filtration. Gao et al. (2020)
PVDF/3D CNTs/MCU- RhB degrade 10.18% RhB degrade 62.50% - 3D built membrane. Shi et al. (2020)
C3N4/GO RhB
Fe3O4/g-C3N4/PVDF - 75% (blending system) 96.7% (magnetic - magnetically induced freezing casting method. Li et al. (2019a)
system)
PAN/SiO2@TiO2 MB 86.1% (blended 99.8% - increased TiO2 surface content of PAN-based membranes by Zhang et al.
membranes) hydrolysis process of SiO2 nanoshells. (2021e)
PVDF/2D/3D g-C3N4/ TC 94.6% (for g-C3N4/BiOI/ 84.0%. (for g- - synergistic effects of Z-scheme 2D/3D g-C3N4/BiOI Cui et al. (2021)
BiOI β-phase PVDF) C3N4/BiOI) heterojunction.
a) Individual photocatalysis (untreated system); b) hybrid photocatalysis (treated/changed system).
that the degradation of certain pesticides remains neglected and usage of interaction between the surface of the membrane and the modi
efficient green photocatalytic techniques is awaiting. fying material (coating materials and some materials can be
Some recent PMs used for the degradation of pesticides under light cross-linked in situ onto the membrane surface).
irradiation are listed in Table 4. (b) Durability. This is an important but poorly investigated quali
The efficiency of a photocatalytic process is governed by many pa tative parameter of photocatalytic composite membranes. Re
rameters (catalyst dosage, dye concentration, pH, presence of other searchers evaluate this parameter from studies of different
ions/species in the reaction mixture, light intensity, etc.), which makes characteristics during long-term usage, including mechanical
it difficult to determine the most efficient system for degrading a stability of the modified and neat membrane (Veréb et al., 2019),
pollutant. However, from the numerous experimental data in the liter changes of photocatalytic activity in time (repeated filtration and
ature, it is possible to evaluate the optimal conditions for improved UV irradiation, after several cycles of photocatalytic treatment
applications. (Hampel et al., 2018; Neghi et al., 2019), modifications in
turbidity (Kovács et al., 2018), rejection rates (the stability after
20 cycles of filtration followed by solar irradiation) (Du et al.,
6.4. Performances of photocatalytic membranes for water purification 2019) and photocatalytic decomposition rate even after 5 cycles
(Liu et al., 2012). Very important and useful from an application
The performance of a membrane depends on numerous factors, perspective would be to find a general technique and optimal
including the design of photocatalytic membrane, pore structure, size, conditions for increasing the durability for different classes of
polarity, roughness, hydrophilicity and mechanical characteristics. Most photocatalytic membranes, but this remains a challenge for
often, the efficiency of a photocatalytic membrane system is measured research.
by the degradation rate of the targeted contaminants and membrane (c) Morphology/structure and design of PMs. Different morphol
flux. Also, good performance of PMs depends on several operating ogies (e.g. nanowires, nanorods, nanocolumns, nanofibers and
conditions, such as the location of photocatalysts (solubilized/sus nanoparticles) of the photocatalyst induce various photocatalytic
pended and immobilized, Section 4), photocatalyst type and its prop performances due to the number of active facets, distinct active
erties (Section 4.1.2), light source (see Section 5). Moreover, sites, and associated adsorption–desorption ability of reactant
photocatalytic membranes prepared using different methods have (Djurišic et al., 2020). For instance, recently, Han et al. (2021)
distinct characteristics such as membrane flux, pollutant degradation prepared an alveoli-like bilayer Janus membrane that has
efficiency, selectivity and anti-fouling performance (Wang et al., air-liquid-solid triphase interfaces with high-efficiency solar-
2017a). The fouling features of the membrane with photocatalysts sus driven and reactive oxygen species generation. Designing pho
pended in the solution are great compared to those of the membrane tocatalytic membranes with excellent photocatalytic and
where the photocatalyst is entrapped or deposited into a template. Other self-cleaning abilities based on the synergistic effect between
common strategies for improving photocatalytic performance are the crystal structures of membrane matrix (Cui et al., 2021).
maximization of light absorption and charge transfer at the surface and (d) Membrane flux. Recently, a multifunctional and flexible Pd
reducing recombination by achieving efficient charge separation and decorated polydopamine - SiO2/PVA electrospun nanofiber
maximizing surface redox reactions. membrane (Yin et al., 2020) showed a high flux (up to 8000 L
Other main features of PMs that need to be investigated for obtaining m− 2 h− 1).
their excellent applicative performances are described below: (e) Degradation rate of the targeted contaminants. The degra
dation rate of the contaminants depends on the various experi
(a) Stability of PMs, under UV irradiation and oxidative envi mental parameters (dose of catalysts, illumination sources,
ronment: Here, there can be appeared and discussed numerous catalyst lifetime etc.) and especially at the experimental illumi
reactions that can occur between the polymer and the incident nation conditions. Therefore, in many studies, the degradation
photons (degradation, functionalization, polymerization, or rate is reported as comparative results obtained by different
isomerization). Among the many polymeric membranes, such as research groups.
PVDF, PC, PS, PTFE, PP, PAN, PES, and CA, were found that
PTFE, PVDF, and PAN membranes were stable even after 30 days In summary, some recent methods used for enhancing the photo
of UV illumination (Chin et al., 2006), showing better perfor catalytic efficiency for the degradation of different pollutants from
mance. Over time, numerous modification methods (e.g., mem water are presented in Table 5.
brane surface modification (surface coating, grafting, and Practically, the performance of PMs can be discussed in terms of
blending) (Miller et al., 2017), influences the stability of the removing and degrading various pollutants in water. Performances of
material added to the membrane. The stability of the photo PMs depend on the nanoparticle composition and concentration,
catalytic membrane can be enhanced by increasing the
11
Fig. 5. Limitations and various ways/techniques for improving the photocatalytic activity/performances of a PMs.
physicochemical properties of metallic nanoparticles (i.e., their shape level) is still scarce (Rasheed et al., 2020). The treatment of wastewater
and surface properties) and other effective factors/parameters of me at a pilot-scale (pre-commercial production system) or even at an
dium mentioned and as can be discussed in Section 5. However, finding industrial-scale level is necessary (Sathya et al., 2021). Since 2005, Ryu
the effective joint between optimal surface properties, its durability, its et al. (2005) characterized and investigated the performance of a
high photocatalytic activity (even under solar irradiation) and cost- pilot-scale photocatalyst-membrane hybrid reactor with 500 L volume
efficiency is another challenge. To date, various attempts have been for the removal efficiency of various micropollutants in water (e.g.
made to improve the photocatalytic activity of the PM, as can be seen in 4-chlorophenol) and concluded that the real applications of this system
Fig. 5. should depend on the treatment cost. Castilla-Caballero et al. (2018)
Recently, Rani and Karthikeyan (2020) reported the optimization of reported evaluation, modelling, and scaling-up of photoreactors using
operational parameters for enhancing acenaphthene degradation by TiO2P25 as catalyst settings for photocatalytic degradation of commer
UV-TiO2 slurry photocatalytic membrane reactor and using response cial acetaminophen. They showed that pH = 9, and a catalyst load of 0.6
surface methodology modelling having Design-Expert software that al g/L are favourable conditions for scaling purposes in this case. Recently,
lows a feasibility study of acenaphthene degradation and an analysis of Gomes et al. (2021) evaluated the impact of Degussa P25 and N–TiO2 on
the effect of operating parameters. insecticide abatement in the water at a pilot-plant scale. The Degussa
P25 has been an excellent solution at the scale of the pilot plant and
7. Efforts for scaling-up of the photocatalytic membranes from ozone under solar radiation increases the photocatalytic activity of
laboratory scale to pilot-plant and commercial level N–TiO2. Moreover, a large photoreactor diameter enhances degradation
with a small quantity of the photocatalyst. Moreover, Wang et al.
Despite a large number of studies regarding the removal of many (2021a) reviewed and analyzed engineering considerations, such as
contaminants from aqueous matrices at the lab level, its application in operation, cost analysis, patents, and several industrial applications of
real wastewater treatment at full scale (at the industrial/commercial the photocatalytic reactors for water treatment. They analyzed and
12
Fig. 6. Schematic diagram of the scaling up process of the photocatalytic membranes (a) laboratory-scale PMs (Zheng et al., 2017), Copyright 2017 MDPI, Basel,
Switzerland; (b) pilot plant (Plakas et al., 2016), Copyright 2016 Elsevier B.V.; (c) industrial scale solar photocatalytic water treatment (Wang et al., 2021a)
Copyright 2021 Elsevier Ltd.
13
discussed the design criteria of photocatalytic reactors for water treat (a) low photocatalytic activity - desirable solar light induced photo
ment, sunlight and artificial radiation sources, the advance in the catalysis membrane;
development of pilot and full-scale photocatalytic water treatment, as (b) membrane fouling (this problem causes damage to the membrane
well as the process economics of these systems. by affecting its permeability, selectivity and reducing its life,
Although intensively studied at the laboratory and pilot level, there especially due to inorganic pollutants that cannot be degraded by
are no industrial/commercial wastewater treatment systems based on photocatalytic membranes);
photocatalytic membranes, the main limits being related to the activa (c) reusability, long-term stability;
tion of solar radiation photocatalysts and the efficiency of continuous (d) associated economic costs (efforts necessary to design and develop
flow processes at the industrial level. Therefore, thanks to those dis the PMs);
cussed above and to the numerous specific characteristics of photo (e) large-scale usage of photocatalytic membranes in practical
catalysis and membranes that have attractive features for water applications.
treatment, expect soon as the photocatalytic membranes to be scaled for
a commercial-scale implementation for water treatment. To date, attempts have been made to mitigate these issues through
A diagram of the scaling up process of the photocatalytic membranes the development of nanocomposite membranes, surface modifications,
is represented in Fig. 6. self-cleaning process (photocatalytic oxidation), feed pretreatment,
An economic feasibility evaluation of the photocatalytic membranes membrane modification, optimization of operating parameters and
is an important issue for evaluating the applicability of the system and membrane cleaning. Further mitigation of the above-mentioned limi
the feasibility for its scaling up. For example, recently, Wang et al. tations further advance the scientific and practical benefits of water
(2021a) presented an exhaustive review for the process economics of decontamination. Specifically, new strategies with more efficiency,
photocatalytic reactors at the pilot scale used for water treatment, which higher economics, and focused on scaling up are highly desirable in the
includes cost study on engineering and set-up, capital cost, labor cost, future.
and annual maintenance, chemical supplies, and treatment cost. The
authors present a review for estimating the operation and capital costs of Declaration of competing interest
different pilot-scale photocatalytic water treatment systems and
conclude that these costs depend on the target contaminant, photo The authors declare that they have no known competing financial
catalyst dose, irradiation source and reactor volume. Although the interests or personal relationships that could have appeared to influence
economic impact of the energy and environmental impact has been the work reported in this paper.
discussed, their implementation on a large scale (industrial/commercial
level) remains limited (Molinari et al., 2021). Acknowledgements
8. Conclusions and perspectives This work was supported by a grant of the Ministry of Research,
Innovation and Digitization, CNCS/CCCDI – UEFISCDI, Romania, proj
In this review, we have discussed advances in the development of ect number PN-III-P1-1.1-TE-2019-0594, within PNCDI III.
photocatalytic membranes, with particular emphasis on their applica
tions in the degradation of pollutants in water. It is noted that numerous Appendix A. Supplementary data
operational conditions, such as reactor design, light intensity, the dose
of the photo-catalyst, organic pollutant, pH and the presence of ions Supplementary data to this article can be found online at https://doi.
affect the photocatalytic membrane processes. This paper reports a wide org/10.1016/j.jenvman.2022.114817.
variety of photocatalytic membranes that can be used in different
operational conditions even though not all of these materials have been References
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Journal of Environmental Management 311 (2022) 114817

Contents lists available at ScienceDirect

Journal of Environmental Management

High-performance photocatalytic membranes for water purification in

pollutants, even at low concentrations in a few hours, without forming

preparation process of the photocatalytic membranes. Recently, Liu Table 1

Table 2 Table 2 (continued )

Fig. 3. Degradation of various dyes using

Fig. 4. (a) Photocatalytic degradation of

TiO2-rGO methomyl complete degradation; 25 min irradiation Luna-Sanguino et al. (2020)

PVA/TiO2 MB 56% 73% - plasma treatment. Montallana et al.

a) Individual photocatalysis (untreated system); b) hybrid photocatalysis (treated/changed system).

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