Separation and Purification Technology 313 (2023) 123517

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Separation and Purification Technology

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Short Communication

Effects of photocatalysis using a photocatalytic concrete board on water

qualities and microbial communities in the aquaculture wastewater
Xu Zhang a, b, c, Li Zhou a, b, *, Min Cai a, b, Naxin Cui a, b, Guoyan Zou a, b, Qian Wang d
a
Eco-Environmental Protection Research Institute, Shanghai Academy of Agricultural Sciences, Shanghai 201403, China
b
Shanghai Engineering Research Centre of Low-carbon Agriculture, Shanghai 201403, China
c
State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
d
Technical Centre for Ecology and Environment of Soil, Agriculture and Rural Area, Ministry of Ecology and Environment, Beijing 100012, China

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

Keywords: A concrete board coated with a composite photocatalyst (tea polyphenols reduced P25/Ag3PO4) was applied in
Concrete board the aquaculture wastewater treatment. The photocatalytic oxidation inhibited algal growth significantly and
Photocatalytic reaction decreased the chlorophyll-a concentration by 60.66%. Meanwhile, organic matter was degraded and the nitrogen
Aquaculture wastewater
form was changed during photocatalytic processes. The variations in nutrients and organic matter after the
Water quality
Microbial community
photocatalytic reaction affected the microbial communities resulting in the aquaculture environment changes.
The photocatalytic reaction did not increase the acute toxicity of the treated aquaculture water as indicated by a
luminescent bacterium. This study provided new insights into the feasibility of employing photocatalytic
oxidation as a realistic method for aquaculture wastewater treatment.

1. Introduction Photocatalytic technology is effective for aquaculture wastewater

treatment. However, in various research on photocatalytic technology
Aquaculture is a rapidly expanding industry as a means to keep pace applications, the purified single pollutant is often used as the research
with population expansion and rising demand for aquatic products [1]. object for targeted problem analysis and investigation, while ignoring
One of the major negative aspects of aquaculture practices is the the impact of the complexity of the actual water environment on the
wastewater laden with remaining feed and feces which can cause severe water remediation. Therefore, the conclusion may not be suitable for the
nutrient and organic pollution [2]. In China, many aquaculture facilities characteristic analysis and pollution control in the actual water envi­
withdraw natural water as the source water and discharge the used ronment. On this basis, this study takes the actual aquaculture water as
water or wastewater back into the source water body. This aquaculture the common research object, to ensure the scientific application of
wastewater discharge may contain nutrients and emerging contami­ photocatalytic technology.
nants that can cause many environmental problems. Therefore, it is The goal of this study was to evaluate the use of a concrete board
imperative for sustainable aquaculture to properly treat the discharged coated with modified P25/Ag3PO4 (T-P25/A), as the visible-light
wastewater and prevent negative impacts on surrounding aquatic responsive photocatalytic catalyst for real aquaculture water treat­
ecosystems. ment. We monitored the levels of organic matter, nutrients, microbial
Photocatalytic technology is a promising approach that utilizes solar community, and toxicity of water after photocatalysis treatment over 20
energy to power water treatment [3]. One of the primary advantages of days. The relationships between water qualities and microbial commu­
photocatalytic reactions is the consumption of minimal or no chemical nity were investigated and the healthy aquaculture environment
agents in the removal of aqueous contaminants [1]. The photocatalytic improvement was finally discussed. This short communication of pho­
treatment was demonstrated as having the ability to degrade organo­ tocatalytic technology in actual aquaculture water has laid the foun­
nitrogen compounds and oxidize ammonia-N causing no significant dation for field implementation and has provided important information
biological impacts on the cultured species [4,5]. Photocatalytic tech­ for a rational design and operation.
nology can also effectively inactivate and destroy a wide spectrum of
microorganisms, including bacteria [6], viruses [7], and fungi [8].

* Corresponding author at: Eco-Environmental Protection Research Institute, Shanghai Academy of Agricultural Sciences, Shanghai 201403, China.
E-mail address: [email protected] (L. Zhou).

https://doi.org/10.1016/j.seppur.2023.123517
Received 16 January 2023; Received in revised form 26 February 2023; Accepted 28 February 2023
Available online 4 March 2023
1383-5866/© 2023 Elsevier B.V. All rights reserved.
X. Zhang et al. Separation and Purification Technology 313 (2023) 123517

2. Methods and materials Material.

2.1. Photocatalytic concrete board preparation and experimental setup 2.4. Microbiome structure analysis

Details regarding the concrete board preparation, experimental Microorganisms in the aquaculture wastewater were collected and
setup, and the original water qualities of aquaculture wastewater were subjected to 16S rRNA gene high-throughput sequencing analysis. The
provided in Text S1 of Supplementary Materials. Briefly, the photo­ details for the bacterial DNA isolation, amplification, sequencing, and
catalytic experiments were performed by placing the concrete board bioinformatic analysis were provided in Text S1 of Supplementary Ma­
coated with the photocatalyst (T-P25/A) in the bottom of a plastic box terial. A Student’s t-test or Welch’s t-test was used for statistical analysis
reactor(480 mmx350 mmx250 mm). White LED lamps with visible-light by SPSS 19.0 (SPSS, Inc., Chicago, IL, USA). Levels of significance are
spectra within 400–780 nm were used to provide irradiation on the top denoted as * p < 0.05, ** p < 0.01, *** p < 0.001, and not significant (n.
of both the control and treatment groups. The schematic diagram of the s.).
experimental setup is shown in Fig. 1. Each box reactor contained 25 L of
aquaculture water with an approximate depth of 15 cm for the control 3. Results and discussion
group and an approximate depth of 16 cm for the treatment group due to
the cement board. White LED lamps with visible-light spectra within 3.1. Characterizations of photocatalytic concrete board
400–780 nm were used to provide irradiation on the top of both the
control and treatment groups. The distance between the lamp on the top Fig. 2(a) shows a picture of a photocatalytic concrete board after
of the reactors and the liquid surface in the reactors was 18 cm with a spraying photocatalysts on the surface of the concrete board. Fig. 2(b, c)
light intensity of 2000 Lux imposed onto the water surface. Two reactors shows the SEM images of the photocatalytic concrete board surface and
(one from the control group and one from the treatment group) were cross-sectional views. The photocatalysts were attached to the concrete
placed side by side on each shelf tier, as shown in Fig. 1. The water board surface which was highly porous and rough. An obvious dividing
samples were collected on days 0, 5, 10, 15, and 20 for analysis of levels line existed in the cross-section of the photocatalytic concrete board.
of organic matter, nutrients, and acute toxicity. For microbial commu­ Below the dividing line, the dense concrete board showed no pores or
nity analysis, three replicate samples were taken from the original gaps. Above the dividing line, the solid with the rough surface exhibited
aquaculture wastewater first (as CT). Three replicate samples were then irregular stacking. The XRD patterns of the P25, T-P25, and T-P25/A
taken from the control group (as C) and treatment group (as T) sepa­ were shown in Fig. 2(d). The diffraction peaks of P25 and T-p25 are
rately after 20 days of the test for comparisons, respectively. consistent with the standard pattern of anatase TiO2 (JCPDS No.
21–1272) and rutile TiO2 (JCPDS No. 21–1276), indicating the mixture
2.2. Chemicals and analytical methods of anatase and rutile TiO2 for P25 and T-P25. The pattern of the com­
posite T-P25/A indicated the presence of Ag3PO4 with a body-centered
Details regarding the chemicals and analytical methods were pro­ cubic structure (JCPDS No. 06–0505), anatase TiO2, and a small portion
vided in Text S1 of Supplementary Material. The details of the analysis of rutile TiO2 in the composite T-P25, respectively. The quantitative
were provided, including the parameters of scanning electron micro­ phase analysis was calculated from the integrated intensities of the
scope (SEM), X-ray diffraction (XRD), fluorescence excitation-emission (1 0 1) peak for the anatase phase and the (1 1 0) peak for the rutile phase
matrix (EEM), inductively coupled plasma-mass spectrometry (ICP- using the reference intensity ratio (RIR) method [9]. It was calculated
MS), and the measurements of chlorophyll-a (Chl-a), total nitrogen (TN), that the anatase/rutile ratio increased to 77.9/22.1 after tea polyphenol
nitrate (NO–3), nitrite (NO–2), ammonium (NH+4 ), total phosphorus (TP),
reduction in the T-P25 from 72.6/27.4 in the P25. The anatase/rutile
total organic carbon (TOC), chemical oxygen demand (COD), absor­ ratio in the T-P25/A was unchanged. The details of T-P25/A charac­
bance at 254 nm (UV254), dissolved organic matter (DOM). teristics have been elaborated on in our previous study [10].

2.3. Acute toxicity assay for the aquaculture wastewater 3.2. Effects on water qualities

The acute toxicity test was conducted with the luminescent bacte­ The Chl-a concentration can better reflect the algal growth and has a
positive correlation with algal cell amounts in water bodies [11]. Fig. 3
rium Vibrio qinghaiensis sp.-Q67 (Q67) as the indicator organism using a
96-well microplate. The details regarding the measurement and calcu­ (a) shows that the Chl-a content of the control group continued to in­
crease within 20 days, whereas the increase in Chl-a content for the
lation of inhibition ratios were provided in Text S1 of Supplementary
treatment group slowed down and leveled off after 10 days. The pho­
tocatalytic oxidation inhibited algal growth significantly and decreased
the Chl-a concentration by 60.66%. Fig. S1 shows the color of the control
group was significantly greener than that of the treatment group. Algae
flocs also adhered to the bottom and walls of the reactor in the control
group after 20 days. This study exhibited that photocatalytic oxidation
can inhibit phytoplankton including algal cell overgrowth in aquacul­
ture water.
The photocatalytic degradation of natural organic matter in aqua­
culture water is also evident as indicated by the change in UV254, COD,
and TOC values (Fig. 3(a)(b)). In the treatment group, the UV254
decreased during the first 5 days and then increased to a steady level
from 5 to 20 days. UV254 is a kind of hydrophobic aromatic organic
matter, which would consume less energy than other organic matter
using photocatalytic technology [12]. It indicated that the hydrophobic
fraction of organic matter was removed faster resulting in UV254
decreased during the first 5 days in the treatment group. With increasing
COD and TOC, the efficiency of UV254 degradation decreased and,
Fig. 1. Schematic diagram of the experimental setup. meanwhile, the released algal organic matter increased UV254

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X. Zhang et al. Separation and Purification Technology 313 (2023) 123517

Fig. 2. (a) The picture of the concrete board with photocatalysts; SEM images of the (b) top view and (c) cross-section of the photocatalytic concrete board surface;
(d) XRD pattern of P25, T-P25, and T-P25/A.

concentration [13] after 5 days of reaction. During the first 5 days, the photocatalytic technology could not degrade organic matter signifi­
concentrations of COD and TOC increased rapidly in the treatment cantly. Using the UV-LED TiO2-photocatalysis in a drinking water
group which are higher than that in the treatment group. On one hand, it reservoir, the treatment units were deployed for 7 days and suppressed
was due to the release of intracellular substances of algae cells after cyanobacterial abundance by 85%, while at the same time, the organic
applying photocatalytic algae inactivation technology. On the other matter showed little significant differences compared with the control
hand, the COD increased because photocatalysis transformed organic group [20].
molecules from those that are resistant to dichromate oxidation in the Inorganic nutrients exhibit obvious impacts on phytoplankton
COD test to those that can be oxidized by dichromate [14]. Due to the growth and aquaculture conditions, thus the concentration changes of
photocatalytic oxidation in the aquatic environment, the COD and TOC inorganic nitrogen nutrients were investigated during the photocatalytic
concentrations showed overall downward trends during the 5–20 days process for 20 days (Fig. 3(c-d)). It was found that the concentrations of
reaction. After 20 days of reaction, the concentrations of UV254, COD, TN were significantly higher than that in the control group due to the
and TOC in the treatment group were 60.92%, 56.42%, and 69.23% of inhibition of algal cells for nutrient absorption in the treatment group.
that in the control group, respectively. However, the nitrogen form conversion occurred in the treatment group
The results of EEMs in Fig. S2 confirmed the organic matter decrease (Fig. S3). The TP concentration was decreased significantly in the
in the treatment group. The peaks in region A at the excitation wave­ treatment group which was consistent with the previous studies [21].
lengths (>250 nm) are related to soluble microbial byproducts and
humic-like organics. The peaks in region B at excitation wavelengths
(<250 nm) are related to aromatic proteins such as tyrosine and fulvic- 3.3. Effects on microbial communities and relationships with water
like materials [15]. The intensities of the EEMs increased as the con­ qualities
centrations of DOMs in the control group increased from 0 to 20 days.
However, the intensities of EEMs in the treatment group changed Except for algae killing or inhibition using photocatalytic technol­
slightly from 0 to 20 days. Through comparison of control and treatment ogy, extensive research has been carried out for the efficient inactivation
groups, the DOMs in the water can be degraded effectively to maintain it of microorganisms [22]. It should be evaluated whether photocatalysis
at a relatively low level by the photocatalytic treatment in aquaculture affects the microbial community of aquaculture water. As shown in
water [15–17]. Table S1, the changes in the Sobs, Chao, ACE, and Shannon indexes (p <
On one hand, the inhibition of algal cells in the treatment group 0.01) indicated a decrease in the richness and diversity of the commu­
reduced the secretion and release of algal organic matter [18]. On the nity. The Venn diagram of Fig. S4 reveals that at the OTUs level, 279
other hand, the photocatalysis in the treatment group resulted in the common core OTUs were shown in CT and C groups. However, only 119
degradation of organic matter [19]. In the other findings, the OTUs were shown in the CT and T groups. 230 and 21 unique OTUs were
distributed in the control and treatment groups, respectively. In general,

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X. Zhang et al. Separation and Purification Technology 313 (2023) 123517

Fig. 3. Time-dependent changes of (a) Chl-a, and UV254, (b) COD, and TOC, (c) TN, and (d) TP.

photocatalytic degradation decreased the microbial diversity of the positive correlation with TN, NO3_N, NO2_N, and the control group
aquaculture water. showed a strong positive correlation with TOC and a slight positive
Fig. 4(a) shows changes in community compositions at the phylum correlation with NH4_N. The most abundant Proteobacteria and Bacter­
level. For the co-existing phyla in both groups, the most abundant oidota correlated positively with TN, NO3_N, and NO2_N. TN is signifi­
phylum was Proteobacteria with an abundance of approximately 55.84% cantly correlated with the bacterial community (p < 0.05). The most
in the control group and 58.28% in the treatment group, respectively. significantly decreased three phyla, Actinobacteriota, Verrucomicrobiota,
Bacteroidota was also one of the important bacterial phyla that slightly and Patescibacteria, all showed positive correlations with TOC. The
changed from 28.98% in the control group to 36.18% in the treatment changes in community composition at the genus level and the correla­
group. There were three kinds of phyla, including Verrucomicrobiota, tion between environmental variables and the bacterial community at
Actinobacteriota, and Patescibacteria, decreasing significantly (p < 0.05) the genus level were shown in Fig. S5.
after photocatalysis. Fig. 4(b) shows the correlation between environ­ It has been known that microbes have a direct or indirect influence
mental variables and the bacterial community. The first two axes of on the aquaculture environment and the health and growth of cultured
redundancy analysis (RDA) explained 63.41% and 28.80% of the vari­ species [23]. It was notable that the increase of subphylum α-Proteo­
ation in the data, respectively. The treatment group showed a strong bacteria and the decrease of subphylum γ-Proteobacteria occurred after

Fig. 4. (a) Relative abundances of bacterial communities at the phylum level. (black asterisks indicated significantly decreased phyla in the treatment group. * p ≤
0.05); (b) RDA of the bacterial community at the phylum level.

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X. Zhang et al. Separation and Purification Technology 313 (2023) 123517

photocatalysis in this study. The increase of γ-Proteobacteria in the

rearing water of fish larvae was associated with lower larval growth
survival, while the predominance of α-Proteobacteria appeared to be a
good indicator of successful larval production [24,25]. The significantly
decreased Verrucomicrobiota and Actinobacteriota in this study correlated
with the healthy aquaculture of yellow grouper (Epinephelus awoara)
[26]. Through the above analysis of microbial community and water
qualities, a preliminary conclusion can be drawn that photocatalytic
technology is beneficial to maintain a healthy aquaculture environment.

3.4. Effects on the water toxicity and reusability of the photocatalytic

concrete board

Relative studies showed that there are substances such as nitrogen-

containing byproducts and cyanotoxins result in increased water
toxicity during treatment processes [27,28]. Photobacterium Q67 has
been proven very useful in evaluating the toxicity of environmental
Fig. 5. The inhibition ratio on Q67 of aquaculture water in control and treat­
pollutants [29]. Fig. 5 indicates that the inhibition ratios on Q67 in the
ment groups.
control group increased significantly from − 1.3% to 24% within 20
days, which is maybe due to the continuous loadings of released or
secreted organic matter induced by the overgrowth of algae and bacte­ administration. Qian Wang: Resources, Project administration.
rium [30]. Conversely, the treated aquaculture water yielded negligible
inhibition ratios, implying toxin degradation by photocatalytic re­ Declaration of Competing Interest
actions. On the other hand, the toxicity due to the released metal ele­
ments from photocatalytic materials should be a concern during water The authors declare that they have no known competing financial
treatment processes. The concentrations of dissolved Ti and Ag were 64 interests or personal relationships that could have appeared to influence
± 3.5 μg/L and 16 ± 1.2 μg/L in the treated aquaculture water after 20 the work reported in this paper.
days of reaction, which complied with the standards for surface water
(GB 3838–2002) and drinking water (GB5749-2006). Based on the Data availability
above results, it can be indicated that the introduction of a photo­
catalytic concrete board did not increase water toxicity. Data will be made available on request.
After 20 days of reaction, the photocatalytic concrete board was
applied twice. The second application was carried out after the complete Acknowledgment
washout of the first, and the aquaculture water was taken from the same
pond with similar water quality. The photocatalytic concrete board This research was financially supported by the Natural Science
exhibited no apparent decrease in inhibition of algal growth. Compared Foundation of Shanghai (No. 21ZR1456700), the Shanghai Sailing
with the control group, the chl-a concentrations in the treatment groups Program (No. 21YF1440900), the National Natural Science Foundation
were decreased by 56.34–62.78%. Meanwhile, the concentrations of of China (No. 42007147), and the National Key Research and Devel­
dissolved Ti and Ag at the second time were 42 ± 2.6 μg/L and 13 ± 0.9 opment Program of China (No. 2021YFC3201503).
μg/L in the treated aquaculture water after 20 days of reaction, which
were less than that at the first time. The above results confirmed the Appendix A. Supplementary data
stability of the photocatalytic concrete board.
Supplementary data to this article can be found online at https://doi.
4. Conclusion org/10.1016/j.seppur.2023.123517.

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