Science of the Total Environment 835 (2022) 155482

Contents lists available at ScienceDirect

Science of the Total Environment

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

Review

Historical development and prospect of intimately coupling photocatalysis

and biological technology for pollutant treatment in sewage: A review
⁎
Kai Liu, Junfeng Chen , Fengfei Sun, Yanyan Liu, Meizhen Tang, Yuewei Yang
⁎
School of Life Sciences, Qufu Normal University, Qufu 273165, PR China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• The progress of photocatalyst, microor-

ganism and carrier in ICPB was summa-
rized.
• The synergistic mechanism of
photocatalysis and biodegradation in
ICPB was described.
• The advantages of ICPB in the degradation
of emerging pollutants were highlighted.
• The further development of ICPB system
was proposed.

A R T I C L E I N F O A B S T R A C T

Editor: Huu Hao Ngo Through the synergistic effect of photocatalysis and biodegradation, intimately coupling photocatalysis and biological
(ICPB) technology could improve the removal rate and mineralization rate of refractory pollutants and reduce the tox-
Keywords: icity of intermediate products. ICPB system was characterized with the advantages of simple operation, low energy
Intimately coupling photocatalysis and biological consumption and high treatment efficiency. As a new sewage treatment technology, ICPB system has shown great po-
(ICPB)
tential in the treatment of refractory pollutants, and has been widely concerned. In this study, the research progress of
Photocatalysis
Biodegradation
photocatalyst, carrier and biofilm in ICPB system were discussed, and the degradation mechanism was introduced. The
Refractory pollutant shortcomings of the current ICPB system were pointed out, and the possible research directions of ICPB in the future
were proposed. This review aimed to deepen the understanding of ICPB technology and promoted the further devel-
opment of ICPB technology in the treatment of refractory pollutants.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Advances in photocatalysts, microorganisms and carriers for ICPB system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1. Improvement of photocatalysts for ICPB system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1.1. Enhancement of ICPB system by modification of TiO2 photocatalyst . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.1.2. Improvement of ICPB system by Bi-based photocatalyst . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.1.3. Improvement of ICPB system by g-C3N4 photocatalyst . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.2. Improvement of microorganisms for ICPB system. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.2.1. Bacteria . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6

⁎ Corresponding authors.
E-mail addresses: chenjunfeng@qfnu.edu.cn (J. Chen), yangyuewei@163.com (Y. Yang).

http://dx.doi.org/10.1016/j.scitotenv.2022.155482
Received 2 April 2022; Received in revised form 17 April 2022; Accepted 19 April 2022
Available online xxxx

0048-9697/© 2022 Elsevier B.V. All rights reserved.

K. Liu et al. Science of the Total Environment 835 (2022) 155482

2.2.2. Fungus . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
2.2.3. Microalgae . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
2.3. Carriers of ICPB . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
2.3.1. Polyurethane sponge . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
2.3.2. Biomass material . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
2.4. Mechanisms of ICPB . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
3. Applications of ICPB . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
3.1. Treatment of municipal wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
3.2. Degradation of heavy metals. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
3.3. Degradation of emerging organic pollutants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
3.3.1. Degradation of polycyclic aromatic hydrocarbons (PAHs) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
3.3.2. Degradation of antibiotics. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
3.3.3. Dye degradation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
3.3.4. Degradation of phenolic compounds . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
4. Problems and prospects of ICPB system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
CRediT authorship contribution statement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14

1. Introduction photocatalysis and biotechnology improved the degradation potential of re-

With the rapid development of urbanization and industrialization, a
large number of pollutants has been released into the environment, which
caused serious influence on the ecological environment and human health
(Manisalidis et al., 2020; Xu et al., 2020). In previous studies, microorgan-
isms has been proved to play an important role in degrading pollutants
(Zhang et al., 2021a, b, c, d). Microorganisms could promote the degrada-
tion of toxic pollutants by releasing different types of enzymes, thus could
degrade them into simpler and less toxic products (Punetha et al., 2022).
The biodegradation methods used to treat these pollutants had the advan-
tages of simple operation, low cost, less secondary pollution, environmental
friendliness and safety (Bhatt et al., 2021; Saravanan et al., 2021). How-
ever, biodegradation was depended on microbial growth and metabolic ac-
tivities, microbial adaptation to pollutants, and chemical properties of
pollutants, as well as nutrients, oxygen concentration, pH value and tem-
perature in the environment, which had a great influence on microbial
growth and metabolism. Therefore, it was difficult for bioremediation to
degrade newly emerging pollutants with high concentration and complex
structure (Premnath et al., 2021; Zhang et al., 2022). Therefore, how to
maintain the advantages of biological treatment technology and combine
it with new sewage treatment technology to achieve effective degradation
of refractory pollutants has become a current research focus.
In order to compensate for the insufficient ability of microorganisms to
deal with refractory pollutant, photocatalysis could decompose refractory
pollutant quickly, so photocatalysis technology was introduced into the bio-
remediation process (Cai et al., 2019a). Photocatalysis used solar energy to
stimulate strong oxidizing substances generated by semiconductor
photocatalysts to degrade pollutants (Hou et al., 2021; Sheng et al.,
2020). When the photocatalyst was photoexcited, the electron-hole pair
in the valence band (VB) of the photocatalyst was separated, and the elec-
tron (e−) was excited to the conduction band (CB), left a hole (h+) in the
VB. The e− and h+ were further reacted with exogenous substances (such
as O2 and H2O) to produce reactive oxidizing species (ROS) such as •O− 2 (Zhong et al., 2021a). Under the protection of the carrier, microorganisms
and •OH (Djellabi et al., 2019; El Mragui et al., 2021). The generated ROS
and h+ were particularly good at attacking double and resonance bonds
in aromatic hydrocarbons, thus achieving ring opening and chain breaking
in organic compounds, so that refractory organic pollutants could be trans-
formed into biodegradable intermediate products (Al-Mamun et al., 2019;
Chávez et al., 2020; Chen et al., 2020a, b, c, d). However, the disorderly,
rapid and indiscriminate chemical reaction of photocatalysis usually leaded
to the accumulation of toxic by-products and excessive residue of oxidation
products, which could not achieve complete mineralization of refractory
pollutants (Fu et al., 2021a; Long et al., 2020). The combination of
fractory pollutants, and biological components could further degrade inter-
mediates induced by photocatalysis (Qin et al., 2020a).
However, the traditional idea was that photocatalytic reaction and bio-
logical treatment were difficult to be carried out in the same reactor, be-
cause the activated substances generated in the photocatalytic process
would inhibit the growth of microorganisms (Waghmode et al., 2019).
Therefore, the photocatalytic reactor should be separated from the biolog-
ical reactor. This sequential coupling process of photocatalysis and micro-
bial treatment technology were named as the independent sequence of
photocatalysis and biodegradation (ISPB) (Lu et al., 2022). However, on ac-
count of the rapid reaction and non-selectivity of photocatalysis, the prod-
ucts of photocatalytic oxidation could not be guaranteed to be
biodegradable in the sequential coupling system, and excessive oxidation
of organic compounds and toxic products might occur in the photocatalytic
process. Toxic or non-biodegradable intermediates produced by
photocatalysis might have adverse effects on the growth and metabolic ac-
tivities of microorganisms, thus poison the bioremediation process and
cause a waste of resources (Chen et al., 2020a; Yu et al., 2020).
However, if photocatalysis and biodegradation occur simultaneously,
this could overcome these problems in ISPB treatment. This new way of
photocatalytic degradation and biodegradation working together was
called intimately coupling of photocatalysis and biodegradation (ICPB).
The concept of ICPB was first proposed by Marsolek et al. (2008), the
basic principle of the technology was that through placing photocatalysts
on the surface of porous carriers such as sponges, honeycomb ceramics
and sodium alginate, microorganisms were evenly distributed in the
pores of the carrier. Under the irradiation of the light source, the
photocatalyst on the surface of the porous carrier was activated, the refrac-
tory pollutant was converted into biodegradable products by the active ox-
idizing species, and the generated intermediate products were then
decomposed again by microorganisms inside the carrier, so as to achieve ef-
ficient degradation and complete mineralization of pollutants in sewage
remained active under attack from ultraviolet light, mechanical forces of
water flow, or free radicals. Therefore, ICPB system could integrate the ad-
vantages of photocatalysis and biodegradation, and solve the problem that
photocatalytic reaction and biological treatment were difficult to be carried
out in the same reactor (Wang et al., 2019a, b, c, d). Recent conclusions
showed that ICPB system performed better than ISPB in the treatment
rate and mineralization rate of refractory pollutants (Liang et al., 2021a).
A number of articles were published and the citation frequency of ICPB
system were shown in Fig. 1a. In the past 18 years, as a new pollutant treat-
ment technology, ICPB system degradation of pollutants began to rise,

2
K. Liu et al.
Fig. 1. (a) Number of articles published on topic of photocatalysis and biodegradation from 2004 to 2022 and citation frequency of ICPB system; (b) The evolution of ICPB
system with time (Web of Science Core Collection).
especially in recent years, more and more studies were focused on ICPB sys-
tem for pollutants degradation. So far, ICPB technology has shown excellent
performance in treating organic pollutants, and many efforts has been made
to improve its efficiency. As was shown in Fig. 1b, the clustering time map
could visually display the research progress in this field and provide direc-
tion for researchers' further research. It was eager to know what were the
bottleneck of photocatalysis and biodegradation for water treatment tech-
nology. And the understanding of the conditions and mechanisms in real-
world environments was still limited by ICPB. Therefore, it was necessary
to prepare this review, hoping to provide theoretical understanding and
new insights for the analysis of ICPB systems, and contributing to the future
development of ICPB.
2. Advances in photocatalysts, microorganisms and carriers for ICPB
system
With the development of reactors, carriers, photocatalytic materials and
biofilms, ICPB has shown increasing potential in the treatment of organic
pollutants (Li et al., 2021a; Zhou et al., 2017). A total of 59 papers were re-
trieved on ICPB system from Web of Science, and Cite Space was used for
keyword analysis (Fig. 2). It could be found that researchers have gradually
deepened their research on ICPB. In recent years, ICPB system, as a new and
excellent sewage treatment technology, has attracted extensive attention of
many scholars (Table S1). In order to improve the processing efficiency of
ICPB system, a new photocatalyst with better catalytic activity should be
prepared firstly, then microorganisms had strong adaptability to the
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Science of the Total Environment 835 (2022) 155482
environment, and finally the porous carrier tightly encapsulated
photocatalyst and microorganisms with good mass transfer effect (Zuo
et al., 2021).
2.1. Improvement of photocatalysts for ICPB system
In ICPB system, photocatalytic reaction was a key step in the process of
converting refractory pollutants into biodegradable intermediates. The se-
lection and properties of photocatalysts were affected by the excitation en-
ergy of photogenerated electrons, and the photocatalysts were excited by
different light sources which had different effects on ICPB system. In addi-
tion, as was shown in Fig. 3, due to the different band gap energy of
photocatalysts, the activity of electrons and holes excited by different
types of photocatalyst was different, leading to different main reactive oxi-
dizing species for photocatalytic degradation, which affected the ability of
ICPB system to deal with refractory pollutants. Hence, the selection and
performance of photocatalyst were key steps for the degradation of pollut-
ants in ICPB system. In early studies, photocatalysts used in ICPB system
were all excited by ultraviolet light (Li et al., 2012; Yan et al., 2013). How-
ever, Zhou et al. (2015) found that the ICPB system under visible light had a
better treatment effect on phenol containing wastewater than the ICPB sys-
tem under ultraviolet light. Because the absorption of ultraviolet light by mi-
croorganisms caused cell membranes to break down and cells to die.
However, under visible light irradiation, the microbial community in the car-
rier was well protected, and the secretion of extracellular polymer was also
enhanced. Therefore, ICPB research could achieve higher degradation effi-
ciency of some refractory pollutants mainly through photocatalysis and
K. Liu et al.
Fig. 2. The keywords analysis of published papers for ICPB system.
microbial degradation induced by visible light. This new ICPB method had a
good ability to mineralize pollutants, protect biofilms, improve solar energy
utilization efficiency and reduce treatment costs (Wang et al., 2019a, b, c, d).
2.1.1. Enhancement of ICPB system by modification of TiO2 photocatalyst
Titanium dioxide (TiO2) was the most common semiconductor
photocatalyst, and it had great potential to mitigate stubborn wastewater
pollutants (Arfanis et al., 2017; Athanasekou et al., 2017). However, it
had a large band gap and low utilization rate of sunlight. Secondly, electron
hole pair of TiO2 was easy to recombine, resulting in reducing photocata-
lytic activity and limiting its application in the treatment of difficult-to-
degrade pollutants (Athanasekou et al., 2018). As the most widely used
photocatalyst, TiO2 has always been a non-negligible photocatalyst selec-
tion scheme in the construction of ICPB system. Ag and Au could be used
as visible photosensitizers of TiO2, and modification of TiO2 by deposition
of precious metals could effectively improve the visible light activity of
TiO2 (Wei et al., 2021). Xiong et al. (2017a) prepared Ag-doped TiO2 visible
light catalyst successfully by modifying TiO2 using the method of precious
Fig. 3. The band structures of several common photocatalysts in ICPB system and some typical redox potentials in photocatalysis.
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Science of the Total Environment 835 (2022) 155482
metal deposition. A novel ICPB system was constructed by supporting
Ag/TiO2 photocatalyst and biofilm. In ICPB system, after 29 cycles, 86 ±
1.3% of the tetracycline hydrochloride (TCH) was still removed by
photocatalysis, and the amount of Ag/TiO2 photocatalyst coating did not
reduction. Liu et al. (2022a, b) constructed a new ICPB system by using
CNTs-Ag modified TiO2 as photocatalyst. After modification, the band
gap of TiO2 decreased to 2.72 eV, which enhanced the visible light activity
of photocatalyst and improved the photocatalytic efficiency. The new ICPB
system was used to degrade Congo red wastewater, and the removal rate of
Congo red was improved. When doped with non-metallic elements, O in
TiO2 lattice was partially replaced, which formed a new energy level
above the valence band of TiO2, reduced the band gap width of TiO2, and
significantly increased the visible light catalytic activity of TiO2 (Zhao
et al., 2020). Wei et al. (2019) constructed an ICPB system for the degrada-
tion of toluene, a volatile organic pollutant, N-TiO2 was used as a
photocatalyst. The part of toluene was destroyed by photocatalysis into bio-
degradable intermediates, which were immediately mineralized by micro-
organisms in biofilms, and toluene was degraded by ICPB, and the
K. Liu et al.
degradation rate reached 99%. N-TiO2 photocatalyst could combine with
biodegradation, improve gas-liquid mass transfer rate and toluene degrada-
tion rate, and enhance the removal ability of p-toluene. Yang et al. (2021a,
b) prepared N-TiO2 and Ag-TiO2 photocatalysts by doping sum of non-
metallic elements. A new ICPB system was successfully constructed on the
non-woven cotton fabric supported by microorganisms, N-TiO2 and Ag-
TiO2 photocatalysts. Two new ICPB systems were prepared to treat tetracy-
cline (TC) wastewater respectively to verify the performance of the two
ICPB systems. The degradation effect of TC wastewater by Ag-TiO2-based
ICPB system was better than that by N-TiO2-based ICPB system. Whether
the photocatalytic performance was good or not would directly lead to
the removal efficiency and mineralization rate of degradation pollutants
in ICPB system. Introducing active semiconductor with narrow band gap
width into TiO2 to form heterojunction was considered to be an effective
method to improve visible light absorption and enhance electron hole
pair separation (Rajendran et al., 2022). Zhang et al. (2020a) prepared
TiO2/g-C3N4 photocatalyst by means of semiconductor recombination,
TiO2/g-C3N4 was supported by in-situ cultured biofilms on spongy carriers
with high porosity, and a new ICPB system was successfully constructed for
reducing nitrate in water. ICPB system had a good effect on nitrite degrada-
tion, and most of the degradation products were converted to N2. Due to the
superior performance of photocatalyst, the direct contact between microor-
ganisms and nitrite was reduced, and the microbial community structure
was optimized to facilitate denitrification, thus improving nitrate reduction
efficiency and inhibiting undesirable intermediates.
2.1.2. Improvement of ICPB system by Bi-based photocatalyst
Bi-based materials were visible light responsive photocatalysts with ap-
propriate band gap and good performance (Ma et al., 2021). Bi-based
photocatalysts had suitable energy band structure and showed effective
photocatalytic activity for pollutant degradation under visible light irradia-
tion. The unique layered structure of Bi-based semiconductor induced inter-
nal electric field within the layer, promoted photogenerated electron and
hole separation, and accelerated charge carrier transfer, thus promoting
photocatalytic performance (Wu et al., 2020). As an excellent visible light
catalyst, Bi-based photocatalyst was a reliable choice for ICPB system con-
struction. Li et al. (2020) used powder spraying method to attach BiOCl/
Bi2WO6/Bi photocatalyst to the outer surface of polyurethane sponge car-
rier, and constructed a new ICPB system. When the visible light induced
ICPB was used to treat tetracycline hydrochloride (TH), the degradation
rate of TH was 97.2%, and the high survival rate of microorganisms con-
firmed that visible light catalyst provided a friendly environment for micro-
bial culture and survival. This work provided a new way to design ICPB
system with low cost, high degradation efficiency and high stability.
Zhang et al. (2021a, b, c, d) prepared Bi2WO6/CN photocatalyst for semi-
conductor composite heterojunction with g-C3N4 and Bi2WO6. Then, a
new ICPB system was constructed by cultivating biofilms inside the sponge
carrier. Through isomerization, the electron hole transfer efficiency and vis-
ible light absorption capacity of photocatalyst were improved, and the
redox capacity of photocatalyst was enhanced. After adding scavenger, the
degradation efficiency of herbicide was reduced, which proved the redox ef-
fect of photocatalysis in the degradation of pollutants in ICPB system. Ding
et al. (2018) prepared a new ICPB system by using a cheap and efficient
ribbon-like oxygen-rich Bi12O17Cl2 as a photocatalyst wrapping on an ammo-
nia ester sponge carrier. In the ICPB system, photoexcited photoelectrons
could be captured by microorganisms as electron donors to promote the
growth of microorganisms and adjusted the microbial community to adapt
to the surrounding environment, which improved the electron hole separa-
tion of photocatalyst and increased the photocatalytic performance. ICPB sys-
tem improved the degradation efficiency of oxytetracycline photocatalytic
process, and oxytetracycline drug resistance and antibacterial activity inter-
mediates were further degraded within 10 min without accumulation.
2.1.3. Improvement of ICPB system by g-C3N4 photocatalyst
Graphite carbonitrides (g-C3N4) nanomaterials had gradually attracted
the attention of multi-disciplinary fields due to their special physical and
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Science of the Total Environment 835 (2022) 155482
chemical properties, such as large specific surface area, low band gap en-
ergy, excellent electronic properties, abundant functional groups and sur-
face defects (Chen et al., 2020b; Liu et al., 2021a, b). The g-C3N4, which
was sensitive to visible light, has become the preferred material for
photocatalysts due to its low cost, good activity and high chemical and ther-
mal stability (Guo et al., 2022a, b). Based on the superior performance of g-
C3N4, g-C3N4 photocatalyst for the construction of new ICPB system has
been paid attention. In order to improve the efficiency of ICPB system for
the treatment of refractory pollutants, Li et al. (2021b) built a novel ICPB
system for the degradation of ciprofloxacin by using polyurethane sponge
supported with g-C3N4 photocatalyst and mixed culture microorganisms.
The removal rate of total organic carbon (TOC) by ICPB system was 1.57
times than that of photocatalytic degradation. The strong decomposition
of ciprofloxacin by g-C3N4 photocatalyst alleviated the pressure of antibi-
otics on microorganisms inside the carrier, which was beneficial to the
growth and metabolism of microorganisms. Microorganisms promoted
photocatalysis by absorbing the electrons which produced by the
photocatalyst. The synergistic effect of ICPB further enhanced the degrada-
tion of ciprofloxacin and improved the mineralization rate. Shi et al. (2022)
used graphite felt (GF) to wrap CdS/g-C3N4 nanocomposites and biofilms,
and constructed a 3D photocatalyst-microbial interface co-degradation
scheme. Genes involved in p-CP biodegradation, hydrogen metabolism
and extracellular electron transfer were significantly enriched under the
protection of the carrier, which revealed that p-CP photocatalytic biodegra-
dation and efficient utilization of photogenerated electrons were enhanced
at the 3D semiconductor-microbial interface. Liu et al. (2022a, b) used inti-
mately coupled photocatalytic and biodegradation system consisting of
Fe3+/g-C3N4 and biofilms to treat synthetic domestic sewage containing
sulfamethoxazole (SMX). ICPB was superior to single photocatalysis or sin-
gle biodegradation of Fe3+/g-C3N4 in the simultaneous removal of SMX
and chemical oxygen demand (COD). The degradation of SMX was mainly
attributed to the photocatalytic activity of Fe3+/g-C3N4. Increasing the dos-
age of Fe3+/g-C3N4 could improve the removal efficiency of SMX. The mi-
croorganisms in ICPB system maintained high survival rate and metabolic
activity, which played an important role in COD removal.
In addition to the above three excellent photocatalysts of ICPB systems
for treating refractory pollutants, many visible light catalysts for excessive
metal oxides have been used to construct ICPB systems. For example, the
excessive metal oxide Ag3PO4 had narrow bandgap energy (2.43 eV) and
higher electron migration ability, which was considered to be a highly effi-
cient heterogeneous photocatalyst driven by visible light (Al Kausor et al.,
2020). Ag3PO4 photocatalyst played an important role in constructing
ICPB system to treat refractory pollutants. Wang et al. (2019a, b, c, d)
suspended highly efficient degradation of microbial alliance (MC) in the in-
ternal space of microcapsules (MI) and visible light photocatalyst, and
Ag3PO4@Fe3O4 was fixed on the film of MI. A novel ICPB system was con-
structed to degrade polycyclic aromatic hydrocarbon (PAHs). PAHs were
effectively removed under the conditions of visible light photocatalysis
and biodegradation. Through MI immobilization, the adverse effect of
photocatalyst on microorganisms was prevented, the degradation effi-
ciency of intermediate products was improved, and the degradation poten-
tial of reactive oxygen species (ROS) produced by photocatalyst was
released. Cai et al. (2019b) estimated the elimination and mineralization
of typical polycyclic aromatic phenanthrene (PHE) using visible light in-
duced ICPB with Mn3O4/MnO2-Ag3PO4 as photocatalyst. Mn3O4/MnO2-
Ag3PO4 photocatalyst had high surface area, ideal absorption capacity
and high photoinduced electron-hole pair separation efficiency, which
could effectively improve the photocatalytic performance and enhance
the removal rate of phenanthrene in ICPB system under visible light.
2.2. Improvement of microorganisms for ICPB system
In ICPB system, microorganisms were an important part of the simulta-
neous coupling of photocatalysis and biological processes. Biodegradation
was a key step to improve the degradation efficiency of pollutants by min-
eralizing pollutants and releasing the degradation ability of reactive oxygen
K. Liu et al.
species produced by photocatalysis. At present, many studies aimed to
build ICPB biofilm system, some research has shown that the microbial
community structure of the biofilm would change after degradation of pol-
lutants, and develop in a direction which was more advantageous to de-
grade the target pollutants (Li et al., 2021b; Zhang et al., 2020a), but
systematic biofilm types were complex, and bacteria were competitive
with each other (Cheng et al., 2021). This inevitably delayed the degrada-
tion efficiency of ICPB system. In order to improve the efficiency of treat-
ment of refractory pollutants by ICPB system, some studies used various
types of pure strains that could efficiently deal with refractory pollutants
to build the ICPB system (Zhang et al., 2021a, b, c, d).
2.2.1. Bacteria
Rhodopseudomonas palustris (R. Palustris) was a phototrophic purple
non‑sulfur bacterium (PNSB) with one of the most extensive metabolic
functions known among bacteria (Li et al., 2021a, b, c, d, e). The high
adaptability and metabolic diversity of R. palustris to organic compounds
such as aromatic pollutants or plant-derived compounds made it an ideal
application of bioremediation (Wang et al., 2019a, b, c, d). Zhang et al.
(2017) constructed a novel ICPB system with photocatalyst (g-C3N4-P25)
and photosynthetic bacteria was wrapped in calcium alginate micro-
spheres. R. palustris has been successfully proved to play a great role in
the degradation of dyes. These alkyl intermediates generated in the degra-
dation process of ICPB system were degraded and mineralized by photosyn-
thetic bacteria, and the oxidation capacity of free radicals was released,
thus degrading reactive brilliant red (X-3b) significantly. Liu et al. (2022)
constructed a new ICPB system using CNTs-Ag/TiO2 as photocatalyst to
Fig. 4. (a) Bacterial populations in biocatalytic and bio-photocatalytic systems before and after 4 h of operation time (all the data represent mean ± SD, n = 3/system) (Xu
et al., 2017); (b) schematic of the concept underlying how the matrix of the ARB-biofilm conducts photo-generated electrons (Zhou et al., 2018); (c) fungal community
composition (genus) structure before (Initial) and after ICPB system operation (Liang et al., 2022); (d) differences in the metabolism involved in energy metabolism
between algae-BiVO4 group and algae-BiVO4-SM2 group (Chen et al., 2020a, b, c, d).
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closely bind R. palustris. The strong oxidation activity of R. palustris pro-
duced by photocatalyst under light also had a certain effect on the growth
of R. palustris. However, R. palustris had certain resistance and adaptability
to active particles. The biodegradation of photocatalytic products increased
the degradation and mineralization of Congo red wastewater by reducing
the competition of free radicals, thus making the whole degradation process
of Congo red more orderly and efficient.
Bacterial degradation efficiency of alkanes with different chain lengths
was based on substrate selection of alkane hydroxylase (AHs) and bioavail-
ability of alkanes. Acinetobacter strain possessed alkylbenzene AHs, which
had a high ability to degrade alkane compounds (Liu et al., 2021a, b).
Acinetobacter had significant ability to degrade refractory pollutants such
as petroleum and pesticides (Kumar et al., 2021). Xu et al. (2017) estab-
lished a photocatalytic biodegradation system using graphite phase carbon
nitriding (g-C3N4) and oil-degrading bacteria (Acinetobacter sp. JLS1), and
evaluated its effect on the degradation of C16 alkanes. The visible light
photocatalysis-biodegradation system had higher degradation efficiency
of C16 alkanes than photocatalysis and biodegradation alone. The positive
synergistic effect between g-C3N4 and strain JLS1 was due to the fact that
g-C3N4 might promote the absorption of C16 alkanes by strain JLS1 by im-
proving the transcription of alkB gene (Fig. 4a), thus promoting the degra-
dation of C16 alkanes. Zhou et al. (2018) coated N-TiO2 photocatalyst on the
surface of porous carrier, and formed anodic respiratory bacteria (ARB)
film in the hole to form ICPB, and explored the electron transfer relation-
ship between ARB and N-TiO2 photocatalyst. An electron transfer mecha-
nism was proposed in ICPB system using ARB biofilms to transfer the
photocatalyzed electrons to the anode through the extracellular electron
K. Liu et al.
carrier of biofilm matrix (Fig. 4b). This property suggested that ICPB could
be used to anodize refractory pollutants and recovered energy from them.
2.2.2. Fungus
Phanerochaete chrysosporium was a famous white rot fungus that could
produce enzymes that degraded various refractory and toxic organic com-
pounds, and was widely used in the degradation of phenols,
polychlorinated biphenyl, pesticides and a series of refractory organic com-
pounds (Chen et al., 2021). Phanerochaete chrysosporium was confirmed to
improve the stable carbon, nitrogen and phosphorus removal efficiency of
activated sludge (Cui et al., 2021). Liang et al. (2022) prepared visible
light induced ICPB system using TiO2/bagasse cellulose composite as car-
rier and Phanerochaete chrysosporiummixed with activated sludge as biolog-
ical source. The ICPB system had significant degradation effects on the
absorbable organic halogens (AOX), dissolved organic carbon (DOC) and
COD of elemental chlorine free (ECF) bleaching wastewater, with degrada-
tion efficiencies of 95%, 91% and 82%, respectively. Phanerochaete
chrysosporium promoted rapid dominance by bacteria with a competitive
advantage in intermediate-degradation (Fig. 4c). Photocatalysis could de-
compose refractory organic matter into small molecules which were easy
to be degraded by microorganisms, thus reducing the adverse factors of mi-
crobial degradation in ECF bleaching wastewater. Hu et al. (2017) con-
structed a novel ICPB system by encapsulating g-C3N4 photocatalyst and
Phanerochaete chrysosporium with calcium alginate beads. The total organic
Fig. 5. (a–d) SEM images of polyurethane sponge carrier surface (a–b) and core (c–d) of the carrier obtained from the ICPB system at the end of experiment (Liu et al., 2022a,
b); (e–f) SEM images of coated with Bi12O17Cl2 and biofilm of polyurethane sponge carrier (Ding et al., 2018).
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carbon (TOC) was removed and the efficiency of the ICPB system reached
74.99% at 72 h, and the removal performance of almost all organic com-
pounds, especially volatile fatty acids and long-chain hydrocarbons, from
landfill leachate were excellent.
2.2.3. Microalgae
Microalgae were oxygen-evolved organisms that could absorb large
amounts of nutrients (carbon, nitrogen and phosphorus) from wastewater
for their growth and development, and also absorb various toxic and persis-
tent pollutants from wastewater (Singh et al., 2021). Microalgae could
change their metabolism between autotrophic and heterotrophic condi-
tions depending on the availability of carbon or nutrient sources in the en-
vironment, thus introducing flexibility and resistance to different
environments even under extreme conditions (Rempel et al., 2021).
Microalgae provided an alternative for wastewater treatment because of
their excellent biodegradation ability in treating domestic and industrial
wastewater, especially for new pollutants (Lage et al., 2018). Salehi et al.
(2019) combined two kinds of microalgae (Chlorella and Duchenella) with
ZnO photocatalyst to construct a photocatalysis-microbial degradation sys-
tem, which improved hydrocarbon removal efficiency in oil-polluted water.
The addition of ZnO nanoparticles to the microalgae suspension had a syn-
ergistic effect on the removal of hydrocarbons from contaminated water,
especially for common chlorella, as over 85% of hydrocarbons were re-
moved in just 3 days of treatment. In order to improve the degradation
K. Liu et al.
efficiency of antibiotics, Chen et al. (2020a, b, c, d) combined photocatalyst
with microalgae Dictyosphaerium sp. The photocatalytic and microbial deg-
radation system was constructed for the degradation effect of sulfadiazine
(SM2). Dictyosphaerium sp. was activated by BiVO4 catalyst. The increase
of carbohydrate metabolites and activation of the TCA cycle played a cru-
cial role in SM2 removal (Fig. 4d).
2.3. Carriers of ICPB
The carrier was a place to protect the metabolic activity of microorgan-
isms in the ICPB system and deal with refractory pollutants (Xiong et al.,
2017a). The carrier must have a large specific surface area to ensure the
uniformity of adhesion of photocatalytic materials and good adsorption of
pollutants. At the same time, the carrier was needed to have good biocom-
patibility and pore structure to ensure that the microorganism could main-
tain better biological activity inside the carrier and ensure that the
intermediate products generated by the photocatalytic reaction (Fu et al.,
2021b). In recent years, polyurethane absorbent and biomass material
has been widely used as the carrier of ICPB system.
2.3.1. Polyurethane sponge
Polyurethane sponge had good biocompatibility and water absorption,
high porosity and apparent density. This carrier was suitable for the rapid
and stable attachment of microorganisms, and improved the microbial
load (Guselnikova et al., 2020). In recent years, studies on the microbial
degradation of polyurethane sponges have attracted increasing attention
from researchers (Jiang et al., 2021). Polyurethane sponge, as a carrier,
combined with photocatalysis and biodegradation, and the construction
of ICPB treatment of pollutants has been more and more widely used
(Ding et al., 2018; Li et al., 2020; Li et al., 2021a; Zhang et al., 2020b;
Zhang et al., 2021a, b, c, d). Liu et al. (2022a, b) constructed a new ICPB
system using polyurethane sponge cube as the carrier. The average side
length of the polyurethane sponge cube (Fig. 5a–d) was 1.0 cm, the porosity
of the cube was up to 95%, and the specific surface area was 1.6 m2/g. In
addition, the cube had excellent water absorption properties, suspending
in aqueous solution when immersed in water. Biofilms in the ICPB system
Fig. 6. (a–b) SEM images of loofah sponge (Li et al., 2021a, b, c, d, e); (c–d) SEM image of calcium alginate for ICPB system (Wang et al., 2019a, b, c, d).
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maintained stable biological activity, species diversity and richness, and
played an important role in COD removal. Xiong et al. (2018) prepared
ICPB system successfully by combining photocatalyst and activated sludge
on a commercial polyurethane sponge cube with a porosity of 87% as a car-
rier. The addition of easily biodegradable co-substrates (acetate) increased
the metabolic activity of microorganisms in the carrier, leaded to the evolu-
tion of the microbial community, enabling more members to biodegrade
the photocatalytic and bioconversion intermediates. Ding et al. (2018) con-
structed ICPB system using polyurethane sponge with higher porosity as the
carrier. The negative effects of direct contact with toxins and oxidants on bio-
film formation could be avoided due to the protection of the carrier. The
large porosity of the carrier provided an easy transport channel for the sub-
strate (Fig. 5e–f), which improved the degradation efficiency of the interme-
diates in the ICPB system. Fu et al. (2021a) used silane coupling agent (SCA)
to enhance the adhesion between TiO2 and polyurethane sponge carrier and
improve the removal efficiency of smelly substances in ICPB system. This
method formed a uniform and dense TiO2 layer on the outer surface of the
carrier, which was firmly coated on the outer surface of the carrier and
protected the microbial community on the inner surface well. The system
maintained excellent removal efficiency and stability even after several oper-
ating cycles. In addition, with the increasing diversity and abundance of mi-
croorganisms, there were multiple pathways for odor removal and the
accumulation of photocatalytic intermediates was reduced.
2.3.2. Biomass material
The toxicity of 2,4-dinitrotoluene (2,4-DNT) was used in polyurethane
production, which was usually used in ICPB polyurethane carrier, and the
bacteria was with poor compatibility (Li et al., 2021a, b, c, d, e). Biomass
materials had unique porous physical structure and excellent mechanical
properties (Fig. 6a–b), and were mainly used as adsorbents and composites
(Li et al., 2018). Biocompatible and naturally available biomass materials
provided potential alternatives to ICPB carriers. Li et al. (2021a, b, c, d, e)
loaded Bi24O31Br10 photocatalyst onto loofah sponge carrier, a biomass ma-
terial with natural three-dimensional porous structure similar to synthetic
sponge, and cultivated biofilms on loofah sponge carrier to construct new
ICPB system. Compared with polyurethane carrier, the removal rate of
K. Liu et al.
TCH was increased by 6.6% and the salinity was enhanced by 9.2% after
using loofah sponge in ICPB, and almost all the photocatalytic products
were degraded. Loofah sponges provided higher bacterial load densities
and higher microbial activity. In addition, it could regulate bacterial com-
munities to have more favorable members to biodegrade photocatalytic in-
termediates. Yang et al. (2021a, b) prepared a novel ICPB system for the
degradation of tetracycline (TC) by loading photocatalytic materials and
microorganisms onto a non-woven carrier of biomass materials with good
biodegradability and high stability. After five cycles, the TC was degraded
which the removal rate reached 82.9%, indicating that the non-woven sup-
port kept good stability of photocatalyst and biofilm. Xiong et al. (2020)
constructed a novel photocatalyst for the degradation of printing and dye-
ing wastewater by wrapping TiO2 photocatalyst and microorganism with
biomass material bagasse cellulose, which was hydrophilic, biodegradable,
high porosity and large specific surface area. In ICPB system, the porous
structure of the support and TiO2 could be observed to ensure the photocat-
alytic performance of the composite support. Under the protection of the
carrier, the microbial community in the carrier steadily evolved in the di-
rection of removing methylene blue dye bacteria. Wang et al. (2019a, b,
c, d) used calcium alginate mixed with Ag3PO4@Fe3O4 and microorgan-
isms to prepare microcapsules to construct a new ICPB system for polycyclic
aromatic hydrocarbon (PAHs) degradation (Fig. 6c–d). Under the protec-
tion of microcapsules, there was no direct contact between the
photocatalyst and microorganisms, so the photocatalyst had little effect
on the survival of microorganisms in the carrier. The potential of microbial
degradation of PAHs intermediates was released and the degradation effi-
ciency of intermediates was improved.
2.4. Mechanisms of ICPB
As a new technology for the treatment of refractory pollutants, ICPB sys-
tem has attracted more and more attention for its complex degradation
principle. Fig. 7 showed the possible mechanisms in the ICPB system. Po-
rous carriers were loaded with photocatalysts and microorganisms
adsorbed contaminants to the surface. Under the irradiation of light source,
when the light energy absorbed by the photocatalyst was greater than the
band gap energy of the photocatalyst, the photocatalyst was excited, re-
sulted in the separation of electron-hole pairs in the VB of the photocatalyst,
and the electrons were excited to the conduction band (CB), leaving holes
(h+) in the VB (Hitam and Jalil, 2020). The e− and h+ further reacted
with dissolved oxygen in water, and water (H2O) or OH− were further gen-
erates active oxidizing species (ROS) such as •O− 2 and •OH. These ROS fur-
ther reacted with refractory pollutants to destroy complex structures in
Fig. 7. Schematic diagram illustrating principle of ICPB system (Liu et al., 2022a, b).
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Science of the Total Environment 835 (2022) 155482
refractory pollutants and generated intermediates (Liu et al., 2020). Biode-
gradable intermediates were transferred to the interior of the carrier, which
were utilized by microbial metabolic activities and further degraded into
carbon dioxide (CO2) and water to complete the mineralization of pollut-
ants. Due to the disorder of photocatalytic reaction, intermediate products
were utilized by microorganisms, thus improving the removal rate of re-
fractory pollutants by photocatalysis (Fu et al., 2021b; Long et al., 2020).
In addition, the electrons generated by photocatalysis were absorbed by mi-
croorganisms as electron donors, which improved the separation efficiency
of electron hole pairs and the metabolic activity of microorganisms, thus
improving the removal rate and mineralization rate of refractory pollutants
treated by ICPB system (Ding et al., 2018; Li et al., 2021a).
3. Applications of ICPB
With the development of ICPB system, under the synergistic action of
photocatalysis and microorganism, ICPB system has been proved to achieve
rapid and efficient removal of refractory pollutants. So far, ICPB system has
been applied to the removal of a variety of refractory pollutants (Fig. 8),
such as phenolic compounds (Shi et al., 2022), antibiotics (Ma et al.,
2018), dyes (Zhang et al., 2017), heavy metals (Pan et al., 2022), etc. Re-
cent studies on the practical application of ICPB in wastewater treatment
were summarized in Table 1.
3.1. Treatment of municipal wastewater
Traditional activated sludge process has always been the core technol-
ogy of municipal wastewater treatment. However, in the face of the im-
provement of sewage discharge standards, it was increasingly difficult to
maintain the treatment of pollutants that were difficult to biodegrade (Ji
et al., 2020; Zhang et al., 2021a, b, c, d). ICPB system could improve the re-
moval efficiency and mineralization rate of refractory pollutants in munic-
ipal wastewater by using the synergistic effect of photocatalysis and
biodegradation. At present, many studies have proved that ICPB system
showed great potential in the treatment of municipal wastewater, including
ECF bleaching wastewater (Liang et al., 2022), antibacterial agents in do-
mestic sewage and COD (Liu et al., 2022a, b). ECF bleaching wastewater
discharged from papermaking industry was characterized by large dis-
charge, high chroma, high organic content, complex composition and diffi-
cult treatment (Sharma et al., 2020). Moreover, ECF bleaching wastewater
contained refractory organochlorides, which could cause paralysis, nausea,
lung dysfunction, and even heart disease or cancer (Hulin et al., 2020).
Therefore, unreasonable and ineffective treatment of this kind of
K. Liu et al. Science of the Total Environment 835 (2022) 155482

Fig. 8. Chemical structure of pollutants used in degradation of ICPB system.

wastewater would cause water pollution and threaten the human health.
Recently, ICPB system has also been applied to remove ECF bleaching
wastewater (Liang et al., 2021b). Liang et al. (2021b) prepared TiO2-
coated sponge biofilm carriers and constructed an ICPB system for degrada-
tion and mineralization of ECF bleaching wastewater. The removal rates of ad-
sorbable organic halides (AOX), COD and DOC in wastewater treatment by
ICPB system was reached 80.3%, 90.5% and 86.7%, respectively, through
the synergistic effect of carrier adsorption, photocatalysis and biodegradation.
The efficiency was significantly higher than that of single biodegradation and
single photocatalytic treatment. A simple and effective strategy to improve the
degradation efficiency of ECF bleaching wastewater was provided.
SMX was an antimicrobial widely used to reduce inflammation in
humans and livestock. Most SMX could not be metabolized in animals
and were eventually discharged into wastewater treatment plants (Cui
et al., 2020). However, due to the low biodegradability of SMX, conven-
tional biotreatment techniques used in wastewater treatment plants could
not effectively degrade SMX (Zhang et al., 2020a, b, c). As an emerging sew-
age treatment technology, ICPB system was used to treat SMX in domestic
wastewater and has achieved excellent results (Liu et al., 2022a, b). Liu
et al. (2022a, b) used a tightly coupled photocatalytic and biodegradation
system consisting of polyurethane sponge cube wrapped with Fe3+/g-
C3N4 and biofilm to treat synthetic domestic sewage containing SMX. The
SMX and COD were removed by ICPB system, and the degradation rate
reached 96.27 ± 5.27% and 86.57 ± 3.06% respectively under the action
of photocatalysis, biodegradation and carrier adsorption, which was better
than that of single photocatalysis and single biodegradation. This study
would provide an effective strategy for the purification of domestic waste-
water contaminated by SMX.

Table 1
Applications of ICPB for the treatment of organic pollutants.
Photocatalysts Microorganism Carriers Target pollution Performance Ref.

TiO2 Activated sludge Polymeric sponge Chlorine dioxide bleaching AOX removal: 80.3% (Liang et al.,
cubes wastewater DOC removal: 90.5% 2021b)
COD removal: 86.7%
Ag/TiO2 Activated sludge Polymeric sponge Tetracycline hydrochloride (TCH) TCH removal: 70% (Xiong et al.,
cubes COD removal: 66% 2017b)
Fe3+/g-C3N4 Activated sludge Polymeric sponge Sulfamethoxazole (SMX) SEM removal: 96.27 ± (Liu et al., 2022)
cubes 5.27%
COD removal: 86.57 ±
3.06%
Cu/N-TiO2 PAH-degrading bacterial Polytetrafluoroethylene Phenanthrene (PHE) PHE removal: 84.29 ± (Qin et al., 2020a)
1.05%
TOC removal: 70.43 ±
2.04%
Bi12O17Cl2 Microorganisms domesticated by Polymeric sponge Oxytetracycline Oxytetracycline removal: (Ding et al., 2018)
oxytetracycline cubes 94%
CNTs-Ag-TiO2 Rhodopseudomonas palustris Calcium alginate Congo red (CR) CR removal: 93.5% (Liu et al., 2022)
COD removal: 94.3%
CdS/g-C3N4 Activated sludge Graphite felts (GF) P-Chlorophenol (p-CP) p-CP removal: 95% (Shi et al., 2022)
TOC removal: 77%
Ag-GeO2/N-TiO2 Activated sludge Hollow fibers Phenolic compounds DOC removal: 98% (Zhong et al.,
COD removal: 91% 2021b)
g-C3N4 Phanerochaete chrysosporium Calcium alginate Landfill leachate TOC removal: 74.99% (Hu et al., 2017)

10
K. Liu et al.
3.2. Degradation of heavy metals
Heavy metals (HMs) were typical pollutants in sewage. Heavy metals
Cd, Cr, Cu, Ni and Zn might have severe toxic and carcinogenic effects on
life, thus posing a major threat to human health through bioaccumulation
in the food chain (Rai et al., 2019). Therefore, the thorough purification
of heavy metals has become an important subject. Recently, many studies
have proved that ICPB system had great potential in removing heavy metals
from water (Pan et al., 2022; Ye et al., 2021). However, heavy metal pollu-
tion was not existed alone, and joint environmental pollution were often oc-
curred. The joint pollution of heavy metals and antibiotics were often
detected in surface water, which increased the difficulty of purifying
heavy metals (Han et al., 2020). Pan et al. (2022) used molybdenum disul-
fide (MoS2) and cobalt disulfide (CoS2) as photocatalysts, a tightly coupled
visible-light responsive photocatalysis and biodegradation system was pre-
pared for the co-treatment of SMX and Cr(VI). Compared with adsorption
and biodegradation systems alone, the synergistic action of photocatalysis
and microorganisms had a huge advantage in removing co-existing pollut-
ants SMX and Cr (VI) (Fig. 9a). The results of toxicity evaluation, excitation-
emission matrix spectroscopy (EEM)and TOC analysis (Fig. 9b–c) indicated
that ICPB was an effective technique for removing and mineralizing of SMX
and Cr(VI). In addition, organic ligands and HMs form stable heavy metal
complexes through coordination bonds, which further led to increase fluid-
ity of metals in the environment, and the removal efficiency of heavy metals
was hindered due to the stable structure of metal complexes (Shan et al.,
2020). Ye et al. (2021) used a tightly coupled photocatalytic and biodegra-
dation system by using non-woven cotton fabric as a carrier to adopt a new
strategy for efficient removal of copper citrate. After 5 cycles, Cu was de-
graded by ICPB system, and the removal rate could still reach 78% within
5 h (Fig. 9d). The complexation of copper citrate (Fig. 9e) was achieved
through the deposition of Cu0 on the surface of photocatalytic materials
by free radical oxidation and the biosorption of Cu2+ by microorganisms.
Therefore, the synergistic effect of photocatalysis and biodegradation im-
proved the removal of Cu in water.
Fig. 9. (a) Concentrations of Cr(VI), Cr(III) and Cr(total) in the effluent of the ICPB system; (b) the EEM images of the solutions obtained after 3 h of treatment with the ICPB
systems; (c) performance of the TOC removal rates of the various systems (Pan et al., 2022); (d) cyclic performance of ICPB system for Cu-citrate removal; (e) possible
mechanisms for Cu complex decomplexation and Cu recovery by ICPB system (Ye et al., 2021).
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Science of the Total Environment 835 (2022) 155482
3.3. Degradation of emerging organic pollutants
The main characteristics of these new organic pollutants were their en-
vironmental persistence, as well as human health was threatened and bio-
accumulation throughout the food chain was affected. These pollutants
could be classified into different categories, such as pesticides, personal
care products, antibiotics and flame retardants (Teodosiu et al., 2018).
These new contaminants could not be removed by these conventional treat-
ment techniques due to their hydrophobic properties (Yang et al., 2017).
Recently, many studies have adopted ICPB system as a new sewage treat-
ment technology to degrade emerging organic pollutants (Guo et al.,
2022a, b; Liu et al., 2022a, b; Qin et al., 2020a; Zhong et al., 2021b).
3.3.1. Degradation of polycyclic aromatic hydrocarbons (PAHs)
As a group of persistent organic pollutants, polycyclic aromatic hydro-
carbons (PAHs) could be produced from natural processes and anthropo-
genic activities such as coal burning and vehicle emissions. PAHs was
highly carcinogenic, teratogenic and mutagenic, posing a threat to the eco-
logical environment, organisms and human health (Souza et al., 2018).
ICPB system has been applied to the removal of PAHs. Through the syner-
gistic effect of photocatalysis and microbial degradation, PAHs and inter-
mediates were effectively degraded (Cai et al., 2019a; Qin et al., 2020b).
Qin et al. (2020a) used Cu, N-TiO2 as photocatalysts and PAHs degradation
bacteria as biofilms, and constructed a new ICPB system for PAHs degrada-
tion. The removal rate of phenanthrene in ICPB system was reached
84.29% ± 1.05% under visible light, which was much higher than that of
photocatalysis and biodegradation alone. The results showed that
photocatalysis, not microorganism, played an important role in the miner-
alization of phenanthrene. Microorganism promoted the photocatalytic
degradation of phenanthrene by degrading the photocatalytic products.
Cai et al. (2019a) constructed a new ICPB system by wrapping microorgan-
isms in activated sludge with Mn3O4/MnO2-Ag3PO4 photocatalyst by
sponge biological carrier. The elimination and mineralization of typical
polycyclic aromatic phenanthrene (PHE) were estimated using visible
K. Liu et al. Science of the Total Environment 835 (2022) 155482

light. Through photocatalytic oxidation and microbial metabolism, organic
pollutants could be completely degraded and detoxicated into harmless
compounds, with the removal efficiency up to 88.1%. In the three cycles,
the PHE removal efficiency tended to be stable. Qin et al. (2020b) reported
a novel photocatalytic bacterial coupled removal system for the treatment
of PAHs-contaminated water. Cu/N co-doped TiO2 and PAH degrading bac-
teria assembled a coupled photocatalytic and biodegradation system,
which promoted the removal and mineralization of pyrene under different
light sources. The coupling system driven by visible light showed a higher
removal rate than ultraviolet light, because ultraviolet light changed the
structure and composition of the bacterial community more than visible
light, and the functional characteristics of the bacterial community were
changed (Fig. 10a) to avoid damage and degradation of pyrene. The
coupled system with visible light irradiation had great potential in the re-
moval of pyrene and had important practical value.
3.3.2. Degradation of antibiotics
Antibiotics, a class of organic molecules, were often used for the preven-
tion and therapy of diseases concerning bacterial infections (Qu et al.,
2020). With the increasing overuse and abuse of antibiotics, the emergence
of antibiotic-resistant bacteria (ARBs) accelerated the spread of antibiotic
resistance, posing a threat to human health and the ecosystem (Wang and
Zhuan, 2020). Due to the persistence of residual antibiotics, it was difficult
to degrade by conventional biotreatment methods (Kang et al., 2020). In
this case, the treatment of antibiotic wastewater by the new wastewater
treatment technology ICPB system has attracted extensive attention (Guo
et al., 2022; Li et al., 2020; Xiong et al., 2017b). Ma et al. (2018) developed
a simplified kinetic model for the ICPB system constructed with Ag/TiO2 as
photocatalyst to simulate the degradation of target pollutants (TCH) dy-
namics of performance. The TCH and COD removal could be predicted by
kinetic model, and the experimental data of R>0.92 was consistent. The
model confirmed that the biodegradation of ICPB played an important
role in accelerating the removal and mineralization of TCH and its interme-
diates. The developed model accurately predicted the efficiency of ICPB
and revealed the operating mechanism of ICPB (Fig. 10b). Ding et al.
(2018) prepared a new ICPB system by using cheap and efficient ribbon-
like one-channel oxygen-rich Bi12O17Cl2 as a photocatalyst and oxytetracy-
cline acclimated microbial community as a biofilm wrapping on ammonia
ester sponge carrier. In the ICPB system, photoelectrons were allowed to
transfer between the photocatalyst and microorganisms without
supplementing the electron donor or increasing the load rate of the
photocatalyst. Compared with the much higher load rate mentioned
above, the required photocatalyst load rate was significantly reduced to
18.3%, and the degradation rate was 94%. The results provided a new strat-
egy for improving the degradation efficiency of oxytetracycline. Guo et al.
(2022) used polyvinyl butyrate (PVB) to improve the adhesion, uniformity
and stability of TiO2 on polyurethane sponge carrier, constructed a new
ICPB system for degradation of TCH. The optimal operating conditions of
ICPB reactor were 40% carrier volume ratio and 6000 μw/cm2 light inten-
sity. Within these optimized parameters, 98% of TCH and 40% of salinity
was removed. Chen et al. (2020) combined BiVO4 photocatalyst and
microalgae Dictyosphaerium sp for ICPB system under visible light. ICPB sys-
tem was applied to the degradation of sulfadiazine (SM2), a representative
sulfadiazine antibiotic. The degradation efficiency of SM2 by ICPB system
was reached 83%, which was better than BiVO4 alone and Dictyosphaerium
sp alone.
3.3.3. Dye degradation
Organic dyes were widely used in many industries such as textile,
leather, paper, printing, cosmetics and plastics, and water discharged by in-
dustry contains a large number of dyes (Wang et al., 2019a, b, c, d). It could
cause respiratory diseases, skin, eyes and gastrointestinal discomfort,

Fig. 10. (a) The classification and relative abundance of bacterial community functions in different samples (A0 for the initial sample; B for the sample collected from
biodegradation group; UV-MB for the sample collected from photocatalysis + biodegradation group irradiated by UV light; V-MB for the sample collected from
photocatalysis + biodegradation group irradiated by visible light) (Qin et al., 2020b); (b) kinetic models of TCH in ICPB system (Ma et al., 2018); (c) synergetic
photocatalytic degradation and biodegradation mechanism of PDI under visible light (Chang et al., 2022); (d) the possible degradation pathways of Congo red in ICPB system
(Liu et al., 2022a, b). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

12
K. Liu et al.
caused serious harm to human and biological health, and posing a great
threat to the ecological environment (Eltaweil et al., 2021; Yang et al.,
2021a, b). Therefore, Congo red wastewater was needed to be treated
harmlessly before being discharged into the environment. However, the
complex chemical molecular structure of dyes made them highly stable
and resistant to degradation (Shah et al., 2020). Printing and dyeing waste-
water treatment technology was increasingly concerned. At present, many
studies have proved that ICPB system had great potential in the degradation
of dye wastewater. Zhang et al. (2017) constructed a novel ICPB system
with photocatalyst (g-C3N4-P25) and photosynthetic bacteria wrapped in
calcium alginate microspheres. The ICPB system converted the dye to ani-
line and phenol derivatives, and then was attacked by free radicals to
form alkyl derivatives. These alkyl intermediates were eventually degraded
by photosynthetic bacteria, and the oxidation capacity of free radicals was
released, thus significantly degrading reactive brilliant red (X-3b). The re-
moval rate of the dye active brilliant red X-3b by the ICPB system was re-
duced by 94%, and the COD of the synthetic wastewater sample was
reduced by 84.7%, which successfully proved the advantages of the combi-
nation of photocatalysis and biodegradation in wastewater purification.
Xiong et al. (2020) constructed a new ICPB system for the degradation of
printing and dyeing wastewater by wrapping TiO2 photocatalyst and micro-
organisms with bagasse cellulose. The final removal rate of methylene blue
by ICPB was 92.08%, indicated that photocatalysis and microbial synergy
were more effective than photocatalysis or biodegradation alone. Improv-
ing the photocatalytic degradation performance of photocatalyst under vis-
ible light could enhance the metabolic activity of microorganism. Chang
et al. (2022) combined n-type semiconductor perylene di-imide (PDI)
with biodegradation to construct a photocatalytic microbial degradation
system. The ICPB system accelerated the biological decolorization and min-
eralization of methyl orange (MO) under light conditions (Fig. 10c). PDI
and free radicals produced had no significant harmful effects on microbial
survival and microbial community. The MO was degraded by synergistic ef-
fect of microorganisms and photocatalysis, and the degradation efficiency
reached 97.9%. Liu et al. (2022a, b) coupled R. palustris and CNTs-Ag-
TiO2 photocatalyst by porous carrier sodium alginate (SA) to prepare a
novel R. palustris/CAT@SA system. The Congo red was degraded by the sys-
tem obviously, and the removal rates were 93.5% and 94.3%, respectively.
According to GC–MS analysis, Congo red entering the interior of the carrier
was mostly degraded into aromatic hydrocarbon compounds, which re-
turned to the surface through the pores of the carrier and were degraded
into biodegradable substances by photocatalyst (Fig. 10d).
3.3.4. Degradation of phenolic compounds
Phenolic compounds were typical examples of biologically refractory
toxic pollutants present in wastewater from various industries such as fun-
gicides, herbicides and textile production (Dong et al., 2016). Different
types of phenolic pollutants were discharged into the environment, causing
considerable harm to organisms due to their difficulty in degradation and
toxicity (Li et al., 2021a, b, c, d, e). At present, many wastewater treatment
technologies were applied to the degradation of phenolic compounds (Gai
et al., 2021). ICPB system has been applied to the degradation of phenolic
compounds and achieved excellent results (Shi et al., 2022; Zhang et al.,
2021a, b, c, d; Zhou et al., 2015). Shi et al. (2022) combined CdS/g-C3N4
photocatalyst with biofilm, constructed a new ICPB system for
chlorophenol degradation. In the absence of additional electron acceptor/
donor, the chlorophenol (P-CP) and TOC were removed by ICPB system,
and the removal rates were 95% and 77%, respectively, which were far su-
perior to traditional photodegradation and biodegradation systems. Yuan
et al. (2021) prepared a novel ICPB system by combining N-TiO2 photocat-
alytic fiber with microalgae biofilm. The biodegradation of 4-chlorophenol
photocatalytic products enhanced the efficiency of free radical oxidation
and increased photocatalysis. The synergistic effect between photocatalyst
and bioreactor enabled the biofilm to maintain the rapid removal of 4-
chlorophenol while maintaining the growth of microalgae biomass, and
the removal of 4-chlorophenol was about 78 μM/h. Zhong et al. (2021b)
prepared synthesis of novel Ag-GeO2/N-TiO2 photocatalyst combined
13
Science of the Total Environment 835 (2022) 155482
with biofilm and development of a novel ICPB system. The ICPB system de-
graded and mineralized three phenolic compounds in high concentration
rapidly and stably. Phototrophs in biofilms provided O2 for photocatalysis
and aerobic biodegradation of phenols and their photocatalytic products.
Biodegradation of phenols and products minimized the unproductive con-
sumption of hydroxyl radicals, thereby enhancing photocatalysis. The
DOC and COD of phenolic compounds were degraded by synergy of ICPB
system with removal rate of 98% and 91%, respectively.
4. Problems and prospects of ICPB system
Since ICPB was first proposed in 2008, the simultaneous coupling of
photocatalysis and biological processes have attracted much research inter-
est as a promising emerging alternative to water purification, and many re-
searchers have successfully applied the technique to treat a variety of
organic pollutants. In order to further promote the development of ICPB,
we put forward the defects and deficiencies in this field.
In order to minimize inhibition of the bioreactor, the selection of
photocatalysts were strictly limited because photocatalyst with biological
toxicity were not permitted in the ICPB. In addition, the photocatalytic per-
formance of photocatalyst under visible light had a great influence on ICPB
system. The photocatalyst with better performance could produce stronger
e− and h+, thus improving the efficient degradation of pollutants.
ICPB might not be suitable for influent wastewater with high organic
loads. Refractory pollutants could directly contact microorganisms by diffu-
sion before being photodegraded, and high concentrations of some highly
toxic pollutants could disrupt microbial activities. At the same time, if the
organic loading rate of pollutants was too high, it might lead to the exces-
sive growth of heterotrophic microorganisms, resulted in the blockage of
carrier pores protecting microorganisms in ICPB, thus affecting the degra-
dation efficiency of ICPB. Currently, most studies on ICPB only investigated
a single pollutant, but actual contaminated sites often contained multiple
pollutants simultaneously, which might inhibit the activity of biofilms
and reduce the efficiency of the entire system. ICPB system had little re-
search on actual polluted wastewater, which limited its development and
practical application in improving the efficiency of pollutant degradation.
The exact mechanism of ICPB was not well understood, and the com-
plex interaction between system components presents challenged to un-
cover the mechanism of ICPB response. For example, the toxicity
mechanism of intermediate products to microorganisms in biofilms, the
mechanism of electron transfer between photocatalyst and biofilm, what
was the ratio between substrate and refractory compound driven the evolu-
tion of microbial community and improved the degradation efficiency of
ICPB system, etc.
Aiming at the shortcomings of the existing ICPB system, we put forward
the development strategy of the next ICPB system. First, the potential of
emerging photocatalytic materials was explored with good biocompatibil-
ity as the next generation of photocatalysts. Secondly, to excavate environ-
mental microbial resources, new genetic engineering knowledge should be
introduced to screen and amplify the most effective microorganisms to de-
grade pollutants, which could shorten hydraulic retention time and save the
capital cost of reactor design. In addition, future carrier applications
depended on the development of high-strength, biocompatible, porous, re-
peatable and 3D carriers with easy-to-implement synthetic solutions. In ad-
dition, the system configuration was improved to ensure long-term
availability and efficiency of components while keeping operating expenses
low. Finally, advanced spectroscopy, mass spectrometry and microbial
metabolomics were used to analyze the operating mechanism of ICPB sys-
tem.
5. Conclusions
The development of ICPB system has proved the following views:
(1) the selection of photocatalyst was excited by ultraviolet light to visible
light, which reduced the cost of degradation of pollutants in ICPB system
and ensured the metabolic activity of microorganisms; (2) synergistic effect
K. Liu et al.
of photocatalysis and biodegradation, the toxic pollutants produced by
photocatalysis could be biodegraded by microorganisms simultaneously,
thus eliminating the cumulative toxic pressure of the intermediates on mi-
croorganisms and releasing the oxidation activity of free radicals; (3) the
electrons generated by photocatalysis might be utilized by microorganisms,
and the microbial community in the carrier has evolved; and (4) the range
of pollutants gradually became more complex, from the degradation of sin-
gle pollutants to the treatment of complex pollutants, the ultimate goal was
to achieve the large-scale application of ICPB system to remove pollutants
in sewage.
This study reviewed the research progress of strong oxidation
photocatalysts, functional microorganisms and porous carriers in ICPB sys-
tem during pollutant degradation. It could help researchers better under-
standing the development and changes of ICPB system. Future research
directions should focus on the preparation of cheap and efficient
photocatalysts, environmentally adaptable microorganisms and intimately
combined high-strength and biocompatible 3D carriers, which would help
to establish reliable, economical and scalable integrated photocatalysis
and biodegradation technologies in practical wastewater treatment plants.
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.scitotenv.2022.155482.
CRediT authorship contribution statement
Kai Liu: Methodology, Software, Investigation, Writing – original draft,
Writing – review & editing, Supervision, Data curation. Junfeng Chen:
Conceptualization, Methodology, Software, Investigation, Writing – origi-
nal draft, Writing – review & editing, Supervision, Data curation. Fengfei
Sun: Writing – review & editing. Yanyan Liu: Writing – review & editing.
Meizhen Tang: Writing – review & editing. Yuewei Yang: Software, Inves-
tigation, Writing – original draft, Writing – review & editing, Supervision.
Declaration of competing interest
We declare that we have no financial and personal relationships with
other people or organizations that can inappropriately influence our work,
there is no professional or other personal interest of any nature or kind in
any product, service and/or company that could be construed as influenc-
ing the position presented in, or the review of, the manuscript.
Acknowledgement
The authors were very grateful for the financial support provided by the
National Natural Science Foundation of China (no. 31901188), China Post-
doctoral Science Foundation (2021M691850) and Shandong Provincial
Natural Science Foundation (ZR2020QC048 and ZR2019BB040).
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