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: dorneanu.petronela@icmpp.ro, pascariu_petronela@yahoo.com (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
need to be separated from the system. This aspect will promote the
practical use of photocatalytic membranes in water treatment (Zhang
et al., 2014). Here, photocatalysts degrade contaminants from polluted
wastewater generating different reactive oxygen species such as •OH,
O2− , H2O2, and 1O2, which are responsible for the mineralization of
pollutants (Nasir et al., 2020). These reactive oxygen species can oxidize
organic contaminants from water.
The performance of a photocatalytic membrane is strongly influ­
enced by the nature of the component materials, as can be seen in
Table S1. Photocatalytic membranes prepared using different methods
exhibit varied properties in terms of membrane flux, pollutant degra­
dation efficiency, selectivity and antifouling performance (Li et al.,
2014). Over time, there have been many limitations in the use of pho­
tocatalytic composite membranes, but also some recently found solu­
tions to these problems, as can be seen in the Supporting Information.
Numerous research groups have reviewed the recent progress of
photocatalytic membranes, including fabrication and characterization
of TiO2-based photocatalytic membranes (Leong et al., 2014), the
application of photocatalytic membranes for water treatment (Bas­
syouni et al., 2019) and H2 production (Iglesias et al., 2016), factors
affecting membrane performance (Zheng et al., 2017). Compared to
other the previously published reviews, this paper mainly reviews the
materials used to produce PMs, the influence of medium factors on the
photocatalytic activity, and their connection with the performance of
PMs that are used for the degradation of various organic pollutants in
wastewater.
2. Photocatalytic degradation and membrane separation
Generally, the photocatalytic membrane processes consist of a
combination of physical separation by filtration and degradation of
pollutants or antibacterial properties obtained from photocatalysis of a
given system. Thus, as is well known, photocatalytic membranes play a

2
M. Homocianu and P. Pascariu Journal of Environmental Management 311 (2022) 114817

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
separation and photocatalytic degradation. Moreover, these membranes
allow independent control of the separation and photocatalytic char­
acteristics because they do not influence each other.
3. Synthesis of photocatalytic membranes
A great number of photocatalytic membranes have been prepared
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

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M. Homocianu and P. Pascariu Journal of Environmental Management 311 (2022) 114817

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

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M. Homocianu and P. Pascariu Journal of Environmental Management 311 (2022) 114817

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
M. Homocianu and P. Pascariu
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
fillers to the polymer, such as polyvinylpyrrolidone (PVP) (Zangeneh
et al., 2019), polyethylene glycol (PEG), and different inorganic salts
(Song et al., 2014).
5. Factors affecting the photocatalytic degradation of pollutant
materials from water
Although, the photocatalysis process occurs under mild operational
conditions, including ambient temperature and pressure, very few
auxiliary additives, and short reaction times (Molinari et al., 2010), the
photodegradation of organic compounds is highly dependent on
numerous parameters, such as the concentration of substrate, type, and
amount of photocatalyst, the surface area of photocatalyst, the tem­
perature of the medium, the pH of the solution, light intensity and
irradiation time, doping of metal ions and nonmetal of photocatalyst and
substrate.
Among these parameters, the photocatalytic degradation and effi­
ciency of the photocatalytic membranes are highly dependent on some
operational parameters, as discussed below.
Structure and morphology of membranes: The structure and
morphology of membranes have significant impacts on their charac­
teristics and performances.
Photocatalyst loading: The catalyst load depends on each system and
is essential for degradation, but most often with a range between 0.04
and 5.0 g/L. Usually, as the catalyst loading increases the surface area of
catalyst available for degradation and adsorption is increased and the
rate of degradation of dyes and pollutants will also increase (Lei et al.,
2018). The more photocatalyst, the more electron-hole pairs are pro­
duced in the system, which generates more hydroxyl radicals. Initially,
the rate of the photoreactions is proportional to the content of the
photocatalyst from the solution, but also at high photocatalyst concen­
tration, the increased particle-particle interactions lead to surface area
loss by agglomeration. Alternatively, a higher amount of catalyst may
also decrease light intensity, slow reaction kinetics, low efficiency, and
catalyst fouling (by blocking the sites or pores) (Molinari et al., 2010).
The optimum loading of the photocatalyst in the photocatalytic mem­
brane depends on the structure and morphology of the membrane, light
intensity, and the flow rate of water.
Light wavelength and intensity: When setting the process parame­
ters, the bandgap energy to activate the photocatalyst must be correlated
with the wavelength of the light source. Light intensity is responsible for
the photocatalytic reaction rate (Loeb et al., 2019). High efficiency in
the solar spectrum region results in increased photocatalytic efficiency.
For a long time, the most widely used light sources were low-efficiency
UV lamps with UV-A (λmax = 355–365 nm) and UV-C (λmax = 254 nm)
because UV light sources allow for higher photonic flux. Newer many
research groups the use of solar and high-efficiency light-emitting di­
odes (LEDs) as durable irradiation sources (Jallouli et al., 2018; Gao
et al., 2017; Ye et al., 2018; Biancullo et al., 2019). At low light intensity,
6
Journal of Environmental Management 311 (2022) 114817
Fig. 2. A summary of the major factors that affect the photocatalytic degra­
dation of pollutant materials from water.
the rate of the photoreactions increases linearly with the rise in the light
intensity because the electron-hole formation is predominant and the
electron-hole recombination is negligible. Instead, at the intermediate
light intensity, the photoreactions depend on the square root of the light
intensity as the separation and recombination of electron pairs compete
at this point. Moreover, at high light intensities, the reaction rate is in­
dependent of this.
Temperature: Usually, photocatalytic reactions occur at room tem­
perature. Many studies have suggested performing the photocatalytic
process at a temperature between 20 and 80 ◦ C. For example, Mozia
(2010) analyzed and found that the optimum temperature range where
the photodecomposition rate increases are between 20 and 60 ◦ C. At
temperatures higher than 80 ◦ C are unfavorable for photocatalytic
processes, due to the promotion of electron/hole recombination and the
exothermic adsorption of the contaminant has a disadvantage, instead of
in the extremely low temperatures (below 0 ◦ C) as a result of desorption
of compounds from the photocatalyst surface the photocatalytic process
becomes a limited step (Zheng et al., 2017), here increases reactant
absorption.
pH: This parameter plays an important role because it influences the
catalysts aggregation and the surface charge of the catalyst and thus
controls the removal efficiency of the pollutants (Sakarkar et al., 2020).
Determining the optimal pH of the solution will enhance the flow and
reduce membrane fouling.
Dissolved oxygen: It plays an important role in the photocatalytic
system for water treatment. The presence of dissolved oxygen in the
system inhibits electron-hole recombination in the photocatalyst,
increasing mineralization, radical formation and catalyst stability.
Ions: The presence of ions influence positive or negative the rate of
the photocatalytic process. The inorganic ions (Cl− , NO3− , SO42− , CO32−
and HCO3− ) from water decreases photocatalytic activity by scavenging
holes (hCB) and hydroxyl radical (•OH) (Borthakur and Das, 2018).
In addition to the above-mentioned parameters, which influence the
kinetics of heterogeneous photocatalysis, a faster reaction is influenced
by the following process parameters, such as dissolved oxygen, flow
rate, a type of pollutant, concentration of the pollutant, catalyst size
(interfacial surface area), and irradiation time (Sundar and Kanmani,
2020). When the pollutant concentration is high, the surface of the
photocatalyst can be saturated, reducing the photodegradation effi­
ciency of the system and irradiation. For this reason, it is tried con­
ducting catalytic tests under water-relevant experimental conditions,
and at a concentration of contaminants that is similar to that found in
wastewater. The agglomerations of pollutants increase the turbidity
solution, which will reduce the light transmission through the solution
and therefore decrease photocatalysts activity.
Furthermore, the numerous parameters described above have moti­
vated researchers to adapt and develop, recently, some studies on the
M. Homocianu and P. Pascariu Journal of Environmental Management 311 (2022) 114817

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
M. Homocianu and P. Pascariu Journal of Environmental Management 311 (2022) 114817

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
reveals that PAN nanofibers effectively adsorb MB species inside the
nanofibers. Strong relationships between the concentration and degra­
dation of MB open a way for the use of this system in the treatment
application of wastewater containing MB. Another literature study re­
ported the magnetic field-assisted fabrication of the PVDF/Ni co-doped
ZnO membranes (Liu et al., 2020) and having magnetic and photo­
catalytic properties and higher antifouling performance than that of
bare PVDF membranes. These membranes can degrade 50% MB within
105 min at the same time having ultrahigh flux recovery rates (FRR) to
100%, 100%, 83% and 83% for filtration of humic acid (HA), sodium
alginate (SA), bovine serum albumin (BSA) and yeast solutions,
respectively, which are comparable or much better than most of the
literature data.
On the same topic, Pascariu et al. (2021b) prepared membranes
consisting of La3+ doped ZnO nanofibers electrospun on PVDF sup­
ports. The photocatalytic efficiency of PVDF/ZnO:Ln (Sm, La, Er) sys­
tems were evaluated in the photocatalytic degradation of MB and RhB,
under visible light irradiation of a polluted solution. The obtained re­
sults show that these membranes present a good photodegradation
(96.33% for MB and 93.36% for RhB) using the PVDF membrane con­
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
M. Homocianu and P. Pascariu
evidenced that the introduction of 37% ZnO:La on PVDF permits
obtaining an enhanced photodegradation of organic pollutants, such MB
and RhB. Moreover, remarkable photocatalytic stability was observed
after ten cycles (98%) of reuse.
https://www.sciencedirect.com/science/article/pii/S1385894
716315339Rajeswari et al. (2017) studied the degradation of Reactive
Red 11 and Reactive Orange 84 dyes from water by ZnO blended cel­
lulose acetate-polyurethane (CA-PU) membrane compared to pure
CA-PU membranes under different experimental conditions, such as
irradiation time, pH and different initial concentration conditions. The
CA-PU/ZnO membrane exhibits improved photocatalytic activities over
the CA-PU membrane at 40 min UV-light irradiation, with an optimum
pH of 7.
In this section and Table 2, we have highlighted significant progress
in the efficiency of photocatalytic membranes used for the degradation
of organic dyes, operating under different experimental conditions.
Based on the data summarized in Table 2, the best results were obtained
for PMs containing photocatalyst TiO2 (commercially available, repro­
ducible and stable) incorporated in numerous membrane templates,
such as PSF, PCND, PVP, PMMA, PA6, PANI/rGO, PET, PVDF, and PSS.
6.2. Photocatalytic degradation of pharmaceuticals from water
Antibiotics, antiinflammatory, and antimicrobials are well-known
pharmaceutical products from wastewater. Antibiotic residues are
considered a major type of emergent pollutant from water. Based on
extensive literature data (Antoniadou et al., 2021) different types of
antibiotics, (including tetracycline, IBP, ciprofloxacin, sulfamethoxa­
zole, and erythromycin), at high concentrations, in all water sources
were found. Actually, more attention has been paid to
visible-light-driven photocatalysis for degrading antibiotics, as can be
seen in Table 3.
Researchers have reported complete removal of some commonly
used pharmaceuticals such as ibuprofen, naproxen, and cetirizine under
UV light irradiation (Mohamed et al., 2018), within 120, 40, and 25 min,
while the same antibiotics under the action of the visible light irradia­
tion (Uheida et al., 2019) the complete (up 99%) degradation was
achieved within 200, 50, and 90 min, using surface-modified TiO2
nanoparticles immobilized on polyacrylonitrile/multiwall carbon
nano-tubes composite nanofibers.
In the visible light photo-degradation of antibiotics, tetracycline (TC)
is one of the most studied antibiotics. For example, Oseghe and Ofomaja
(2018) using C-doped TiO2 (0.3 g/L) with visible-LED light illumination
(2 h) removed 70% of TC (5.0 mg/L). Recently, Wu et al. (2021) found
that Black TiO2 exhibits much higher TC (66.2%) removal efficiency
than white TiO2 (43.4%). Also, the authors established that TC can be
mineralized by black TiO2 under visible light irradiation, but not by
white TiO2. Instead, in 2021, Luo et al. (2021) using a PVDF photo­
catalytic membrane based on NCQDs/BiOBr/TiO2 heterojunction suc­
ceeded to reach a TC degradation rate of 77% within 120 min, under
visible light irradiation. Also, Zong et al. (2021) fabricate a
photo-response and superwettable NiAlFe LDH/PDA/PVDF membrane
that showed high oil-in-water emulsion separation performance (>99%)
and can effectively degrade tetracycline, within 20 min under UV light
irradiation.
Song et al. (2020b) reported a highly flexible, core-shell hetero­
structured, and visible-light-driven membrane assembled from
g-C3N4@Co–TiO2 and PVP, matrix, which served as excellent photo­
catalytic membranes. These membranes have good reversibility and
recyclability. Advantages of three-dimensional porous networks
enhanced visible-light response induced a prominent photodegradation
efficiency of 90.8% toward tetracycline hydrochloride, after 60 min
visible light irradiation and displayed excellent antibacterial perfor­
mance (E. Coli inactivation after 90 min of visible light exposure). In a
similar study by Song et al. (2020a) a ternary Ag@ZnO/TiO2 fibrous
membrane was used to photodegradation of tetracycline hydrochloride.
9
Journal of Environmental Management 311 (2022) 114817
The presence of Ag nanoparticles induces light absorption, large surface
area, and effective charge separation, and thus this means that prepared
Ag@ZnO/TiO2 membranes exhibited greater photocatalytic degrada­
tion efficiency of 91.6% toward tetracycline hydrochloride within 1 h,
and show prominent antibacterial activity (after 1 h of simulated solar
light exposure). According to www.sciencedirect.com/science/artic
le/abs/pii/S0376738820313247Zhang et al. (2021d) Ti3+-TiO2 photo­
catalytic membranes were prepared by a combination of hydrothermal
reaction and low-temperature vacuum-activation methods and showed
enhanced photodegradation of tetracycline and anti-fouling ability
under visible light irradiation. The improved performance was due to
the high concentration stable Ti3+ centres, which are more active spe­
cies. These photocatalytic membranes displayed 95.9% and 81.2% ef­
ficiency in TC degradation, upon 100 min visible light irradiation and
antifouling ability, for practical wastewater treatment.
More recently, a novel Z-scheme 2D/3D g-C3N4/BiOI-based β-phase
PVDF photocatalytic membranes (Cui et al., 2021) have an exceptional
photocatalytic degradation efficiency for tetracycline (94.6%) compared
with CN/BI heterojunction power (84.0%) and two other control
membrane matrices (CN/BI/PAN and CN/BI/CA PMs) within 120 min.
Recently, a multifunctional nanocomposite membrane Ag–TiO2/
PVDF-HFP (Salazar et al., 2020) was used to degrade norfloxacin under
ultraviolet (UV) and visible radiation. These nanocomposite membranes
with different concentrations of TiO2 and Ag–TiO2 were found to be
photoactive to UV and visible light. The nanocomposites with Ag–TiO2
show the highest degradation efficiencies: 64.2% under UV and 80.7%
under the visible radiation, for 90 and 300 min, respectively. Also,
antimicrobial tests were performed against two bacterial species (gram
+ and gram -).
A photocatalytic system constructed from the NiO/m-TiO2 nano­
composites at different NiO contents (Faisal et al., 2018) showed the
complete degradation of gemifloxacin mesylate (20 mg/L) after 180 min
of visible light illumination. It was observed that it exhibited excellent
photocatalytic performance compared with either pure NiO or m-TiO2
photocatalysts under visible light illumination.
Ibuprofen (IBP) is a pharmaceutical from the class of nonsteroidal
anti-inflammatory drugs typically used for treating fever and inflam­
mation, with low toxicity, higher efficiency, fruitful results that make its
excess usage and become an emerging organic micropollutant. Recent
studies (Singh et al., 2019) have demonstrated that Cu2O photocatalyst
modified PSF matrix membranes prepared using the phase inversion
technique were successfully used to remove IBP under visible light. The
Cu2O photocatalyst exhibits a positive effect on membrane hydrophi­
licity and antifouling nature of the membrane, by improved flux from
34.24 L m− 2 h− 1–179.54 L m− 2 h− 1 and water contact angle decreased
from 71.5◦ to 45.3◦ values. The highest amount of the Cu2O photocat
alyst modified PSF membranes showed efficient removal of IBP under
simulated light and acidic conditions, with a removal rate of 32.63 ×
10− 3 min− 1 and an efficiency of 86%. Simsek (2017) was reported that
IBP was successfully degraded in the presence of boron (B)-doped TiO2
compared to pure TiO2 (removal rates of 85% and 25% for B-doped TiO2
and pure TiO2, respectively), due to the enhanced crystallinity and
electronic properties of TiO2. The effects of g-C3N4/TiO2/Fe3O4@SiO2
heterostructured nanophotocatalyst (Kumar et al., 2018) on the effi­
ciency of enhanced photocatalytic removal of ibuprofen from real
sewage effluent under visible light were investigated. A photocatalytic
performance (97% IBP removal at 15 min of visible light irradiation at
pH 7), from real sewage effluent, was recorded and more than 87%
removal efficiency was maintained even after 3 consecutive recycles.
These aspects indicate the great potential of this system for practical
environmental applications.
Another nonsteroidal anti-inflammatory drug, namely, naproxen
(NPR) exist in excess in surface water, groundwater, wastewater,
seawater and even in drinking water, at concentrations ranging from
10− 1–105 ng L− 1 (Lancheros et al., 2019) and was studied under
UV–visible irradiation. Photocatalysis is one of many methods (e.g.
M. Homocianu and P. Pascariu
adsorption, sono-assisted processes, ozonation, photo-Fenton and
advanced oxidation processes) used to remove naproxen. For example,
Torki and Faghihian (2018) photodegrade NPR using Fe3O4@PPY(pol­
ypyrrole)-NiS, at pH = 7, under visible light irradiation and obtained an
efficiency of 87%, within 30 min. Instead, under similar conditions (pH
= 7, visible light irradiation-lamp 500 W), using the titanate nano­
material, a research group (Fan et al., 2019) failed to degrade 100%
NPR, upon 180 min of irradiation.
Great interest in the potential practical application shows the
degradation of a mixture of antibiotics from wastewater. M-Elefther­
iadou et al. (2019) tested the photocatalytic activity of PET/TiO2 (10%,
30%, and 47% TiO2) systems on the degradation of the antibiotic mix­
tures (Isoniazid, Metronizadole, Sulfadiazine, Sulfamethoxazole,
Trimethoprim, Norfloxacin, Moxifloxacin and Lincomycin, see Fig. 4) in
the water and wastewater matrix. PET-10% wt TiO2 exhibited high
performance even after 5 cycles of reuse and at higher TiO2 loading, the
reusability of the photocatalysts decreased. The results showed that
PET-10%-TiO2 was efficient in degrading the antibiotic mixture in water
as follows: Lincomycin, Moxifloxacin, Isoniazid, Metronidazole and
Norfloxacin were almost completely degraded within the first 2 h of
irradiation, while trimethoprim, sulfadiazine and sulfamethoxazole
required a more prolonged time for complete disappearance (90, 93 and
98% degradation respectively after 6 h of treatment).
Many photocatalytic membranes have been used for the photo­
catalytic degradation of the most consumed antibiotics and anti-
inflammatory drugs (ciprofloxacin, norfloxacin, tetracyclines, nap­
roxen, and ibuprofen) under visible light irradiation. Note that it is
difficult to determine the most efficient PMs used in the photo­
degradation of pharmaceuticals from wastewater, as the reported results
were obtained under different conditions and are mainly limited by the
scale-up of studies from laboratory to industrial scale, the most efficient
reuse of the system and the removal of photocatalysts from wastewater
after treatment.
Table 4
Some recent PMs used for the degradation of pesticides under light irradiation.
PMs Pesticide Target Light source/degradation rate
TiO2-rGO methomyl complete degradation; 25 min irradiation
TiO2/SiC foams paraquat UV-C (254 nm); 91%; 3h
PVDF/PDA- roxarsone ~100%; 3h; visible light
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.
DCP)
10
Journal of Environmental Management 311 (2022) 114817
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.
6.3. Photocatalytic degradation of pesticides from water
Pesticides are the second most dangerous compound water
contaminant among various organic pollutants and represent a signifi­
cant human and environmental risk (Khan and Pathak, 2020). One of the
persistent pesticides from water is Endosulfan (Arisekar et al., 2019).
Many metal-organic frameworks (Cu-MOF, Zr-MOF, Zn-MOF, and
Al-MOF) having a porous structure and highly photocatalytic activity
were used over time to remove several pesticides (Liu et al., 2017a;
Wang et al. 2020a; Ahamad et al., 2020).
In recent years, regarding photo-pesticide degradation, notably,
Ahamad et al. (2020) reported MoS2/ZnS embedded in N/S doped car­
bon for photocatalytic degradation of pesticides. The authors find that
approximately 85% degradation of dicofol was achieved by the nano­
composite photocatalyst and the catalytic activities remain around
77.2% after investigating the stability and reusability via five cycles.
Also, Abdelhameed et al. (2021) employed a Cu-MOF@cellulose acetate
membrane for the selective removal of dimethoate pesticides from
wastewater. These materials also showed high adsorption capacity
(282.3–321.9 mg/g) and good recyclability (the adsorption efficiency of
the membrane was diminished by 22.5%, after 5 reusing cycles). Zhao
et al. (2020) prepared g-C3N4/Ag NPs intercalated GO composite
membrane, which under visible-light irradiation can photocatalytic
degradation of paraoxon-ethyl pesticide. The results showed that 92.8%
of paraoxon-ethyl could be degraded after 150 min visible-light irradi­
ation. Afterwards, Luna-Sanguino et al. (2020) produce TiO2-rGO
nanocomposite materials for solar photocatalytic degradation of pesti­
cides at the pilot plant scale. It can be observed that TiO2 is uniformly
distributed on rGO surfaces forming a network structure. The photo­
catalytic capacity of TiO2-rGO was investigated for the removal of pes­
ticides, including methomyl, pyrimethanil, isoproturon and alachlor, by
using H2O2 or O2 as the oxidants, under solar irradiation at pilot-plant
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
Ref.
Luna-Sanguino et al. (2020)
Marien et al. (2019)
Zhou et al. (2020)
Hoseini et al. (2017)
M. Homocianu and P. Pascariu
Table 5
Recently developed methods used for the enhancement of photocatalytic efficiency for the degradation of different pollutants from water.
PMs/pollutants Photocatalytic response
a) b)
PVA/TiO2 MB 56% 73%
PVP/rGO@TiO2 MO 52.4 mg removed 112.4 mg removed
PVDF/3D CNTs/MCU- RhB degrade 10.18% RhB degrade 62.50%
C3N4/GO RhB
Fe3O4/g-C3N4/PVDF - 75% (blending system) 96.7% (magnetic
system)
PAN/SiO2@TiO2 MB 86.1% (blended 99.8%
membranes)
PVDF/2D/3D g-C3N4/ TC 94.6% (for g-C3N4/BiOI/ 84.0%. (for g-
BiOI β-phase PVDF) C3N4/BiOI)
a) Individual photocatalysis (untreated system); b) hybrid photocatalysis (treated/changed system).
that the degradation of certain pesticides remains neglected and usage of
efficient green photocatalytic techniques is awaiting.
Some recent PMs used for the degradation of pesticides under light
irradiation are listed in Table 4.
The efficiency of a photocatalytic process is governed by many pa­
rameters (catalyst dosage, dye concentration, pH, presence of other
ions/species in the reaction mixture, light intensity, etc.), which makes
it difficult to determine the most efficient system for degrading a
pollutant. However, from the numerous experimental data in the liter­
ature, it is possible to evaluate the optimal conditions for improved
applications.
6.4. Performances of photocatalytic membranes for water purification
The performance of a membrane depends on numerous factors,
including the design of photocatalytic membrane, pore structure, size,
polarity, roughness, hydrophilicity and mechanical characteristics. Most
often, the efficiency of a photocatalytic membrane system is measured
by the degradation rate of the targeted contaminants and membrane
flux. Also, good performance of PMs depends on several operating
conditions, such as the location of photocatalysts (solubilized/sus­
pended and immobilized, Section 4), photocatalyst type and its prop­
erties (Section 4.1.2), light source (see Section 5). Moreover,
photocatalytic membranes prepared using different methods have
distinct characteristics such as membrane flux, pollutant degradation
efficiency, selectivity and anti-fouling performance (Wang et al.,
2017a). The fouling features of the membrane with photocatalysts sus­
pended in the solution are great compared to those of the membrane
where the photocatalyst is entrapped or deposited into a template. Other
common strategies for improving photocatalytic performance are
maximization of light absorption and charge transfer at the surface and
reducing recombination by achieving efficient charge separation and
maximizing surface redox reactions.
Other main features of PMs that need to be investigated for obtaining
their excellent applicative performances are described below:
(a) Stability of PMs, under UV irradiation and oxidative envi­
ronment: Here, there can be appeared and discussed numerous
reactions that can occur between the polymer and the incident
photons (degradation, functionalization, polymerization, or
isomerization). Among the many polymeric membranes, such as
PVDF, PC, PS, PTFE, PP, PAN, PES, and CA, were found that
PTFE, PVDF, and PAN membranes were stable even after 30 days
of UV illumination (Chin et al., 2006), showing better perfor­
mance. Over time, numerous modification methods (e.g., mem­
brane surface modification (surface coating, grafting, and
blending) (Miller et al., 2017), influences the stability of the
material added to the membrane. The stability of the photo­
catalytic membrane can be enhanced by increasing the
11
Journal of Environmental Management 311 (2022) 114817
Methods Ref.
- plasma treatment. Montallana et al.
(2020)
- enhancement of photocatalytic degradation due to filtration. Gao et al. (2020)
- 3D built membrane. Shi et al. (2020)
- magnetically induced freezing casting method. Li et al. (2019a)
- increased TiO2 surface content of PAN-based membranes by Zhang et al.
hydrolysis process of SiO2 nanoshells. (2021e)
- synergistic effects of Z-scheme 2D/3D g-C3N4/BiOI Cui et al. (2021)
heterojunction.
interaction between the surface of the membrane and the modi­
fying material (coating materials and some materials can be
cross-linked in situ onto the membrane surface).
(b) Durability. This is an important but poorly investigated quali­
tative parameter of photocatalytic composite membranes. Re­
searchers evaluate this parameter from studies of different
characteristics during long-term usage, including mechanical
stability of the modified and neat membrane (Veréb et al., 2019),
changes of photocatalytic activity in time (repeated filtration and
UV irradiation, after several cycles of photocatalytic treatment
(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.,
2019) and photocatalytic decomposition rate even after 5 cycles
(Liu et al., 2012). Very important and useful from an application
perspective would be to find a general technique and optimal
conditions for increasing the durability for different classes of
photocatalytic membranes, but this remains a challenge for
research.
(c) Morphology/structure and design of PMs. Different morphol­
ogies (e.g. nanowires, nanorods, nanocolumns, nanofibers and
nanoparticles) of the photocatalyst induce various photocatalytic
performances due to the number of active facets, distinct active
sites, and associated adsorption–desorption ability of reactant
(Djurišic et al., 2020). For instance, recently, Han et al. (2021)
prepared an alveoli-like bilayer Janus membrane that has
air-liquid-solid triphase interfaces with high-efficiency solar-­
driven and reactive oxygen species generation. Designing pho­
tocatalytic membranes with excellent photocatalytic and
self-cleaning abilities based on the synergistic effect between
the crystal structures of membrane matrix (Cui et al., 2021).
(d) Membrane flux. Recently, a multifunctional and flexible Pd
decorated polydopamine - SiO2/PVA electrospun nanofiber
membrane (Yin et al., 2020) showed a high flux (up to 8000 L
m− 2 h− 1).
(e) Degradation rate of the targeted contaminants. The degra­
dation rate of the contaminants depends on the various experi­
mental parameters (dose of catalysts, illumination sources,
catalyst lifetime etc.) and especially at the experimental illumi­
nation conditions. Therefore, in many studies, the degradation
rate is reported as comparative results obtained by different
research groups.
In summary, some recent methods used for enhancing the photo­
catalytic efficiency for the degradation of different pollutants from
water are presented in Table 5.
Practically, the performance of PMs can be discussed in terms of
removing and degrading various pollutants in water. Performances of
PMs depend on the nanoparticle composition and concentration,
M. Homocianu and P. Pascariu
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
and surface properties) and other effective factors/parameters of me­
dium mentioned and as can be discussed in Section 5. However, finding
the effective joint between optimal surface properties, its durability, its
high photocatalytic activity (even under solar irradiation) and cost-
efficiency is another challenge. To date, various attempts have been
made to improve the photocatalytic activity of the PM, as can be seen in
Fig. 5.
Recently, Rani and Karthikeyan (2020) reported the optimization of
operational parameters for enhancing acenaphthene degradation by
UV-TiO2 slurry photocatalytic membrane reactor and using response
surface methodology modelling having Design-Expert software that al­
lows a feasibility study of acenaphthene degradation and an analysis of
the effect of operating parameters.
7. Efforts for scaling-up of the photocatalytic membranes from
laboratory scale to pilot-plant and commercial level
Despite a large number of studies regarding the removal of many
contaminants from aqueous matrices at the lab level, its application in
real wastewater treatment at full scale (at the industrial/commercial
12
Journal of Environmental Management 311 (2022) 114817
level) is still scarce (Rasheed et al., 2020). The treatment of wastewater
at a pilot-scale (pre-commercial production system) or even at an
industrial-scale level is necessary (Sathya et al., 2021). Since 2005, Ryu
et al. (2005) characterized and investigated the performance of a
pilot-scale photocatalyst-membrane hybrid reactor with 500 L volume
for the removal efficiency of various micropollutants in water (e.g.
4-chlorophenol) and concluded that the real applications of this system
should depend on the treatment cost. Castilla-Caballero et al. (2018)
reported evaluation, modelling, and scaling-up of photoreactors using
TiO2P25 as catalyst settings for photocatalytic degradation of commer­
cial acetaminophen. They showed that pH = 9, and a catalyst load of 0.6
g/L are favourable conditions for scaling purposes in this case. Recently,
Gomes et al. (2021) evaluated the impact of Degussa P25 and N–TiO2 on
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
ozone under solar radiation increases the photocatalytic activity of
N–TiO2. Moreover, a large photoreactor diameter enhances degradation
with a small quantity of the photocatalyst. Moreover, Wang et al.
(2021a) reviewed and analyzed engineering considerations, such as
operation, cost analysis, patents, and several industrial applications of
the photocatalytic reactors for water treatment. They analyzed and
M. Homocianu and P. Pascariu Journal of Environmental Management 311 (2022) 114817

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
M. Homocianu and P. Pascariu
discussed the design criteria of photocatalytic reactors for water treat­
ment, sunlight and artificial radiation sources, the advance in the
development of pilot and full-scale photocatalytic water treatment, as
well as the process economics of these systems.
Although intensively studied at the laboratory and pilot level, there
are no industrial/commercial wastewater treatment systems based on
photocatalytic membranes, the main limits being related to the activa­
tion of solar radiation photocatalysts and the efficiency of continuous
flow processes at the industrial level. Therefore, thanks to those dis­
cussed above and to the numerous specific characteristics of photo­
catalysis and membranes that have attractive features for water
treatment, expect soon as the photocatalytic membranes to be scaled for
a commercial-scale implementation for water treatment.
A diagram of the scaling up process of the photocatalytic membranes
is represented in Fig. 6.
An economic feasibility evaluation of the photocatalytic membranes
is an important issue for evaluating the applicability of the system and
the feasibility for its scaling up. For example, recently, Wang et al.
(2021a) presented an exhaustive review for the process economics of
photocatalytic reactors at the pilot scale used for water treatment, which
includes cost study on engineering and set-up, capital cost, labor cost,
and annual maintenance, chemical supplies, and treatment cost. The
authors present a review for estimating the operation and capital costs of
different pilot-scale photocatalytic water treatment systems and
conclude that these costs depend on the target contaminant, photo­
catalyst dose, irradiation source and reactor volume. Although the
economic impact of the energy and environmental impact has been
discussed, their implementation on a large scale (industrial/commercial
level) remains limited (Molinari et al., 2021).
8. Conclusions and perspectives
In this review, we have discussed advances in the development of
photocatalytic membranes, with particular emphasis on their applica­
tions in the degradation of pollutants in water. It is noted that numerous
operational conditions, such as reactor design, light intensity, the dose
of the photo-catalyst, organic pollutant, pH and the presence of ions
affect the photocatalytic membrane processes. This paper reports a wide
variety of photocatalytic membranes that can be used in different
operational conditions even though not all of these materials have been
yet transferred to industrial production. The growing technologies and
population cause main water contaminants and require advanced water
treatment technologies. The photocatalytic process completely degrades
organic pollutants. The PMs have a combination of properties, such as
antimicrobial activity, super hydrophilicity, high photocatalytic oxida­
tion, and separation that allows acting to eliminate and photocatalytic
degradation of the organic pollutants, bacteria, and viruses from water.
PMs are considered green tools due to: the end products of photo­
catalysis are eco-friendly, such as H2O, simple salts, and minerals, no
other oxidants are required for the process (atmospheric oxygen is
enough), the photocatalyst is non-toxic, cost-effective, chemical, and
biologically inert, renewable and reusable, activation of photocatalyst
occurs by the action of sunlight as well as artificial light. Photocatalytic
membranes play a major role in water treatment technologies due to
their incorporation of membrane separation with photocatalysis in a
single unit. Recently, PMs have become emerging innovative products
with great potential to be used at industrial level water purification.
Superhydrophilic photocatalytic membranes are promising for treating
oil contaminated waters because of their simultaneous efficiency in both
degrading and separating organic contaminants from the water.
The use of photocatalytic membranes in water treatment is prom­
ising to show performance on a large scale. Despite the remarkable
performance of photocatalytic membranes, several limitations have
been identified and need to be further explored:
14
Journal of Environmental Management 311 (2022) 114817
(a) low photocatalytic activity - desirable solar light induced photo­
catalysis membrane;
(b) membrane fouling (this problem causes damage to the membrane
by affecting its permeability, selectivity and reducing its life,
especially due to inorganic pollutants that cannot be degraded by
photocatalytic membranes);
(c) reusability, long-term stability;
(d) associated economic costs (efforts necessary to design and develop
the PMs);
(e) large-scale usage of photocatalytic membranes in practical
applications.
To date, attempts have been made to mitigate these issues through
the development of nanocomposite membranes, surface modifications,
self-cleaning process (photocatalytic oxidation), feed pretreatment,
membrane modification, optimization of operating parameters and
membrane cleaning. Further mitigation of the above-mentioned limi­
tations further advance the scientific and practical benefits of water
decontamination. Specifically, new strategies with more efficiency,
higher economics, and focused on scaling up are highly desirable in the
future.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgements
This work was supported by a grant of the Ministry of Research,
Innovation and Digitization, CNCS/CCCDI – UEFISCDI, Romania, proj­
ect number PN-III-P1-1.1-TE-2019-0594, within PNCDI III.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jenvman.2022.114817.
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