Science of the Total Environment 750 (2021) 141510

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Science of the Total Environment

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

Removal of arsenic from water through ceramic filter modified by

nano-CeO2: A cost-effective approach for remote areas
Xiaohan Yang a, Guohe Huang b,⁎, Chunjiang An c, Xiujuan Chen d, Jian Shen d, Jianan Yin d, Pei Song e,
Ziqing Xu a, Yongping Li b
a
State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment, Beijing Normal University, Beijing 100875, China
b
Center for Energy, Environment and Ecology Research, UR-BNU, School of Environment, Beijing Normal University, Beijing 100875, China
c
Department of Building, Civil and Environmental Engineering, Concordia University, Montreal, Quebec H3G 1M8, Canada
d
Institute for Energy, Environment and Sustainable Communities, University of Regina, Regina S4S 0A2, Canada
e
MOE Key Laboratory of Resources and Environmental Systems Optimization, North China Electric Power University, Beijing 102206, 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

• Ceramic filter modified by nano-CeO2

was produced for water purification.
• Influent arsenic concentration and pH
were significant influencing factors.
• As(V) and turbidity in water were re-
moved by CF-CeO2 simultaneously.
• The macro- and microscopic mecha-
nisms of As(V) removal using CF-CeO2
were revealed.
• Using CF-CeO2 is a cost-effective ap-
proach for arsenic removal in remote
areas.

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

Article history: The groundwater with high arsenic concentration is widespread, especially in many remote areas of developing
Received 10 May 2020 countries. Arsenic existing in drinking water sources has a high risk to human health. In this study, an innovative
Received in revised form 11 July 2020 effort to remove As(V) from water using ceramic filters functionalized with CeO2 nanocomposites (CF-CeO2) was
Accepted 3 August 2020
investigated. Considering removal efficiency and flow rate, the suitable coating amount of CeO2 was determined
Available online 4 August 2020
for the production of CF-CeO2. Based on the factorial analysis, influent arsenic concentration and pH were found
Editor: Daniel CW Tsang to be significant factors in As(V) removal. Furthermore, CF-CeO2 exhibited a good removal capability over a wide
pH range and was insensitive to the change of background electrolyte concentration. In the treatment of natural
Keywords: water, the existence of medium and low turbidity levels facilitated As(V) removing, while the high turbidity level
Ceramic filter exhibited the opposite effect. Based on macroscopic experiments and microscopic characterizations, it was re-
Arsenic(V) vealed that the As(V) removal mechanism by the CF-CeO2 mainly included ion-exchange and electrostatic attrac-
Filtration tion. The findings in this study provided convincing evidence for the use of CF-CeO2 as a high-efficiency, low-cost,
Simultaneous removal and safe approach for water purification in the remote areas of developing countries.
Mechanism
© 2020 Elsevier B.V. All rights reserved.
Synchrotron-based analysis

1. Introduction

⁎ Corresponding author at: Center for Energy, Environment and Ecology Research, UR-
Drinking water safety is essential for all human beings (Fang et al.,
BNU, School of Environment, Beijing Normal University, Beijing 100875, China. 2019; Huang et al., 2019; Kot et al., 2015; Schwarzenbach et al., 2010).
E-mail address: huang@iseis.org (G. Huang). In recent years, arsenic contamination in drinking water has attracted

https://doi.org/10.1016/j.scitotenv.2020.141510
0048-9697/© 2020 Elsevier B.V. All rights reserved.
2 X. Yang et al. / Science of the Total Environment 750 (2021) 141510
wide attention (Awual et al., 2019; Khatamian et al., 2017; Wang et al.,
2018a; Yu et al., 2018). Arsenic in water source derives from both an-
thropogenic and natural activities. The groundwater with high arsenic
concentration is widespread, especially in many remote areas of devel-
oping countries (Fendorf et al., 2010). Arsenic existing in drinking water
sources has a high risk to human health. The International Agency for
Research on Cancer (IARC) has identified arsenic as a carcinogen
(Althouse et al., 1979). It was reported that the total population exposed
to arsenic-contaminated water above 10 μg/L, the EPA arsenic standard
for drinking water, could be upwards of 19 million people across China
(Rodríguez-Lado et al., 2013). In Pakistan, much of the Indus Plain is suf-
fering from the arsenic-related health risk with the impact on approxi-
mately 50 to 60 million people using groundwater with excessive
arsenic (Podgorski et al., 2017). Endemic arsenic poisoning caused by
drinking high arsenic water has become a global environmental and
health problem.
In urban areas, centralized water systems are often used to ensure
the water safety of residents (Moeini and Afshar, 2019). However, the
construction and maintenance costs of such treatment and distribution
systems are relatively high. In some developing countries and regions,
due to economic and technical constraints, there is a lack of appropriate
infrastructure and drinking water safety is difficult to guarantee
(Budinova et al., 2006; Liu et al., 2019; Ren et al., 2013; Yao et al.,
2020). According to the characteristics of decentralized residence in
rural areas, the distributed household devices for drinking water treat-
ment are more suitable. For remote areas in developing countries, the
development of efficient and cost-effective household treatment de-
vices is crucial for ensuring drinking water safety.
The ceramic filter is a gravity-driven system without additional en-
ergy requirement. The main materials for making ceramic filter include
clay and rice husk, which are widely available with very low cost (Xu
et al., 2020). Rice husk is agricultural waste and it is sustainable when
such waste can be used as pore-making agent in the fabrication of ce-
ramic filters (Ren et al., 2013). The use of ceramic filters will be of
great significance in improving the safety of drinking water in remote
areas. The research on ceramic filters to date mainly focused on their an-
tibacterial performance. The previous studies have shown that ceramic
microfiltration technology has a good ability to remove bacteria
(Ekpunobi et al., 2019). The ceramic filter with micropore size coated
with nano silver, nano TiO2, and some nanocomposites such as Fe/
TiO2 and Ag/ZnO could inactivate bacteria effectively (Huang et al.,
2020; Kallman et al., 2011; Zhao et al., 2020). However, the studies of
using ceramic filters for arsenic removal are very few. Ceramic particles
coated with nano zero-valent iron could remove arsenic from water
(Robbins et al., 2014). But nano zero-valent iron is unstable and has
low adsorption capacity (Bakshi et al., 2018). It has been proved that ce-
rium oxide has an exceptional capacity for the adsorption of arsenic
(Wang et al., 2018b). As a cheap and abundant rare earth metal oxide,
cerium oxide has very low acid solubility which can limit its loss in
use (Li et al., 2012). Cerium oxide has the good adsorption performance
due to its high porosity and it has been proved feasible to remove arse-
nic using cerium oxide-based materials (Asere et al., 2017; Song et al.,
2020; Yu et al., 2015b). To date, there has been no application of cerium
oxide nanoparticles to modify ceramic filters. The understanding of ar-
senic removal mechanism in filtration and the interactive effect of dif-
ferent environmental factors are also very limited. Introducing cerium
oxide nanoparticles into the ceramic filter through surface modification
can be potentially a high-efficiency, low-cost, and safe approach for
water purification.
Therefore, an innovative effort to remove arsenic using ceramic fil-
ters functionalized with CeO2 nanocomposites (CF-CeO2) will be inves-
tigated in this study. To be specific, (1) the production of CF-CeO2 will be
determined in terms of removal efficiency and filtrated flux; (2) the
morphology and crystal phase of CF-CeO2 will be characterized;
(3) the impact of different conditions including influent arsenic concen-
tration, pH and background electrolyte concentration will be analyzed
through factorial analysis; (4) the performance of simultaneous re-
moval of turbidity and arsenic using CF-CeO2 will be evaluated;
(5) the arsenic removal mechanism of CF-CeO2 will be explored based
on the macroscopic and microscopic analyses. The results can help de-
velop a novel and low-cost arsenic removal device for the rural and re-
mote areas.
2. Materials and methods
2.1. Materials
Clay and rice husk used in the production of ceramic filter were col-
lected from Beijing ZhidaTenghui Trading Company (Beijing, China) and
Happy Farm Feed Factory (Jiangsu, China), respectively. Nano-CeO2
particles (20–50 nm, 99.5%) were purchased from Shanghai Macklin
Biochemical Technology Co., Ltd. (Shanghai, China). Reagent-grade so-
dium arsenate dodecahydrate (Na₃AsO₄•12H₂O) was purchased from
Beijing Chemical Works (Beijing, China) and was dissolved into deion-
ized water to prepare As(V) solution. Turbidity in raw water was
prepared by dispersing kaolin purchased from Sinopharm Chemical Re-
agent Co., Ltd. (Shanghai, China) in deionized water. All other chemicals
were of reagent grade or higher.
2.2. Filtration device
Fig. S1 shows the ceramic filtration system included a synthetic glass
column, two flanges, and a beaker. The upper flange and the synthetic
glass column were one unit. The ceramic filter was held in place be-
tween two flanges. The inner edges of the flanges were sealed with rub-
ber rings to prevent water leaking. Two flanges were connected and
secured using screws. The raw water was poured from the top of the
glass column and flowed through the ceramic filter under the force of
gravity. The middle of the lower flange was a convex cone with the
same diameter as the synthetic glass column. There was a small hole
about 1.0 cm in diameter at the center of the cone. After being filtered
through CF-CeO2, the treated water came out through the hole and
was collected in the beaker. The filtration system was kept in dark dur-
ing the tests. All experimental glass devices were soaked in the dilute ni-
tric acid solution for a few hours in case of the residual of arsenic, then
were washed using deionized water several times before experiments.
2.3. Production of CF-CeO2
Rice husk size has a significant effect on flow rate, further influencing
the removal efficiency and filtration performance (Huang et al., 2018).
Excessive flow rate could reduce the contact time of raw water and
CF-CeO2, which would further lead to a decrease in removal efficiency
(Ali et al., 2019). Nevertheless, too low flow rate would also affect the
filtration performance of CF-CeO2. To ensure consistency and quality
of CF-CeO2, rice husk was sieved (0.15–0.18 mm mesh) before produc-
ing (He et al., 2018). The ceramic filters were made of mixing clay,
sieved rice husk, and deionized water in a certain proportion. The mix-
ture was pressed into a mold to shape a disk with the diameter of
10.0 cm and the thickness of 1.5 cm by press machine. The generated ce-
ramic filters were air-dried at room temperature for 2–3 days and dried
in the oven at 100 °C for two days to evaporate all moisture. Then the
ceramic filters were sintered in a muffle furnace and heated at
1000 °C with a heating rate of 2 °C/min. Nano-CeO2 particles were
added into deionized water. The solution with nano-CeO2 particles
was distributed through ultrasonic dispersion for 20 min followed by
magnetic stirring for 1 h. The ceramic filters were modified by brushing
dispersed nano-CeO2 suspension on the surface and the generated CF-
CeO2 was dried for further filtration.
 X. Yang et al. / Science of the Total Environment 750 (2021) 141510
2.4. Arsenic removal experiments
During the modification of ceramic filters with nano-CeO2 suspen-
sion, the coating amount of nano-CeO2 was ranging from 0.00 to
1.00 g, which was corresponding with the use of 0 to 10 mL dispersed
nano-CeO2 suspension at 0.1 g/mL on the surface of ceramic filter. The
contents of the As(V) in effluent were detected to calculate the arsenic
removal efficiency of CF-CeO2. The flow rate of the filtration device
was represented by the filtrated flux at which 1 L of raw water was fil-
tered. Factorial analysis has often been used in experimental design to
investigated the interactions of multiple factors (Shen et al., 2017;
Song et al., 2018; Xin et al., 2019a; Xin et al., 2019b). A 23 factorial design
was used to explore the significant factors and the interactions of these
factors in water purification. The effects of influent arsenic concentra-
tion (A), pH (B), and background electrolyte concentration (C) were
considered. The arsenic removal efficiency was presented as the re-
sponse. The empirical model was established in the experiment, and
the quadratic model for analysis is shown as follows (Arslan-Alaton
et al., 2009; Rodrigues et al., 2009):
Y ¼ b0 þ b1 X1 þ b2 X2 þ b3 X3 þ b4 X1 X2 þ b5 X1 X3 þ b6 X2 X3
þ b7 X1 X2 X3
where Y is the global mean; X1, X2, X3 are independent variables; bi is
the coefficient matching up with the effects and interactions of the fac-
tors. The value of each factor at different levels is shown in Table S1. The
detailed factual and coded experimental matrix design is shown in
Table 1.
In addition, to investigate the effect of pH on the arsenic removal
performance of CF-CeO2, the pH value was set in the range from 3 to
11. To determine the influence of background electrolyte concentration
on the arsenic removal, the background electrolyte concentration in
aqueous solution varied from 0.001 to 0.100 mol/L. The ionic strength
of these solutions was conducted by sodium nitrate (NaNO3). To evalu-
ate the simultaneous removal performance of turbidity and arsenic
using CF-CeO2, the turbidity in influent ranged from 0 to 200 NTU. Re-
sults were presented based on arsenic removal ratio and influent tur-
bidity. In the above experiments, the initial arsenic concentration was
100 mg/L. All the filtration tests were performed with 100 mL of raw
water. After the treatment of the filtration device, the samples of efflu-
ent were collected.
2.5. Analytical methods
The arsenic concentration in effluent was measured by an atomic
fluorescence spectrophotometer (AFS-9800, Beijing KeChuangHaiGuang
Instrument Inc., Beijing, China). Prior to measurement, the samples
were acidified with 2% concentrated HCl and detected within one day
after collection (Zhang et al., 2013). The performance of CF-CeO2 was
expressed by arsenic removal efficiency. It was calculated by the following
equation:
C0 −Ce
Arsenic removal efficiency ¼  100%
C0
where C0 and Ce are the arsenic concentrations in influent and effluent,
respectively.
The contents of cerium in effluent were measured by a SPECTRO
ARCOS EOP Axial View Inductively Coupled Plasma Atomic Emission
Spectrometer (ICP-AES, SPECTRO Analytical Instruments GmbH, USA).
All filtration experiments were performed at room temperature of
25 °C and in triplicate. The standard deviation (SD) is presented in
graphs. Factorial analysis was conducted using Design-Expert 8.0 soft-
ware (Stat-Ease Inc., USA).
Scanning electron microscope (S-4800 SEM, Rigaku, Japan) was per-
formed to analyze the surface and cross-section structure of CF-CeO2.
The elemental composition of the sample was obtained using EX-350
3
energy dispersive spectroscopy (EDS, Rigaku, Japan). The surface of
CF-CeO2 was coated by platinum in vacuum. The crystal structure of
CF-CeO2 was identified by the D/max-2550 X-ray diffractometer (XRD,
Rigaku, Japan) with Cu radiation at 40 kV and 40 mA over the range
(2θ) of 5–80°. Zeta-potential of CF-CeO2 at different pH levels was ex-
amined by zeta sizer nano ZS90 (Malvern Panalytical Ltd., Malvern,
UK). Fourier transform infrared spectroscopy (FTIR) spectra were mea-
sured by Nicolet Nexus 670 FIIR spectrometer (Thermo Fisher Scientific,
Waltham, USA). The wavenumber was collected from 4000 to 400 cm−1
with a resolution of 4.0 cm−1. The X-ray photoelectron spectroscopic
(XPS) data of samples was recorded by an ESCSLAB 250Xi photoelectron
spectroscopy (Thermo Fisher Scientific Inc., Waltham, U.S.A.) with
monochromatic AlKα radiation (BE = 1486.6 eV) of 500 μm beam
spot. The XPS results were shown as binding energy figures and fitted
through the XPSPEAK41 Software. The synchrotron radiation-X-ray
fluorescence (SR-XRF) mappings and spectra of Ce and As concentration
distributions on cross sections of CF-CeO2 were measured at the Very
Sensitive Elemental and Structural Probe Employing Radiation from a
Synchrotron (VESPERS) beamline located at third generation Canadian
Light Source (CLS) in Saskatoon, Canada. The samples were excited by
the polychromatic X-ray (pink beam), and a Vortex-ME4 4-element sil-
ð1Þ
icon drift detector (SDD) was employed to collect the emitted SR-XRF
spectrum. The reported SR-XRF spectra were based on the average of
SR-XRF spectra of the selected area, and the SR-XRF mapping was plot-
ted by SigmaPlot 14.0.
3. Results and discussion
3.1. Determination of CF-CeO2 production condition
In the use of ceramic filter, both removal efficiency and flow rate are
important indicators of its performance. It is necessary to determine a
coating amount that can not only achieve good arsenic removal effec-
tiveness but also maintain the permeate flow rate within an appropriate
range. As shown in Fig. 1, the amount of nano-CeO2 coated on the sur-
face of ceramic filters had a significant influence on the arsenic removal
efficiency and flow rate of CF-CeO2. The results showed the arsenic re-
moval efficiency increased significantly from 64.04% to 84.58% with
the increase of coating amount from 0.10 to 1.00 g, which was calcu-
lated based on the concentration of nano-CeO2 suspension at 0.1 g/mL
and the volume of suspension solution used in coating. Even without
coating, ceramic filters could also remove 61.93% of arsenic in influent.
After the modification by nano-CeO2, the flow rate decreased sharply.
It was due to the impact that some pores on the ceramic filter surface
were covered by nano-CeO2, resulting in the decrease of flow rate.
With the increase of coating amount, the arsenic removal efficiency
gradually increased, and then the growth rate slowed down, while
there was also a decrease in flow rate. After coating with certain
amount, the growth rate of arsenic removal efficiency was less than
the declining rate of flow rate. The positive impact due to the increase
of the removal efficiency was not enough to offset the negative impact
due to the decrease in flow rate. Thus it was unnecessary to continue in-
ð2Þ creasing the amount of coating. Based on these findings, the 1.00 g
nano-CeO2 was suggested to be a suitable amount on CF-CeO2. After fil-
tration, the cerium concentration in effluent was also measured and no
cerium was detected (the detection limit was 10 μg/L). The determined
CF-CeO2 production conditions would be used in the following tests.
3.2. Characterization of CF-CeO2 filter
Fig. 2 shows the SEM and EDS results of morphology and the chem-
ical compositions in CF-CeO2. On the surface of the ceramic filter with-
out nano-CeO2, the microstructure exhibited a randomly distributed
porous structure (Fig. 2A). The main elements of ceramic filter were O
(51.69%), Si (19.17%), Al (10.70%), C (8.79%). During the sintering pro-
cess, as the temperature increased, the pore-forming materials (rice
4 X. Yang et al. / Science of the Total Environment 750 (2021) 141510

Table 1
Coded levels and corresponding values for factorial design matrix.

Run Number Coded levels A B C

A B C Influent Arsenic Concentration (mg/L) pH Background Electrolyte Concentration (mol/L)

1 1 −1 1 100 6 0.100
2 −1 1 −1 50 9 0.001
3 −1 −1 −1 50 6 0.001
4 1 1 −1 100 9 0.001
5 1 1 1 100 9 0.100
6 1 1 1 100 9 0.100
7 1 1 −1 100 9 0.001
8 −1 −1 −1 50 6 0.001
9 1 −1 −1 100 6 0.001
10 −1 1 1 50 9 0.100
11 −1 1 −1 50 9 0.001
12 −1 1 1 50 9 0.100
13 1 −1 −1 100 6 0.001
14 −1 −1 1 50 6 0.100
15 −1 −1 1 50 6 0.100
16 1 −1 1 100 6 0.100

husk) burned to generate a large number of pores on the surface and in-
side of the ceramic filter (Zhang and Oyanedel-Craver, 2013). Such po-
rous structure of CF-CeO2 had a capacity to seize undesired pollutants
while maintaining the water flowing rate. The surface of the ceramic fil-
ter became rougher after decorating nano-CeO2 (Fig. 2B). The cerium
peaks were shown in the EDS spectrogram of CF-CeO2 with a content
of 7.14%, indicating that the surface of ceramic filters was loaded with
nano-CeO2 particles. The nano-CeO2 particles were homogeneously dis-
tributed on the surface of the ceramic filter, which would ensure the suf-
ficient contact between nanoparticles and raw water. Moreover, the
morphological structure of CF-CeO2 showed no obvious difference
with CF, implying that the modification did not alter the morphology
of ceramic filters. The narrow and winding channels were observed on
the interior cross-section of CF-CeO2 (Fig. 2C). The edge cross-section
of CF-CeO2 was also characterized (Fig. 2D). Comparing the EDS results
of the interior and the edge cross-section, it was shown that no cerium
element was detected in the inner channels, while it largely distributed
at the edge of the cross-section. The results confirmed that nano-CeO2
particles were only loaded on the surface of ceramic filters instead of en-
tering into the interior of ceramic filters.
The XRD patterns of CF, nano-CeO2 particles and CF-CeO2 are shown
in Fig. 3. The narrow peaks suggested that the samples were of the crys-
tal structures. The most abundant crystalline phase in CF and CF-CeO2
were both the quartz which contains silicon and oxygen elements (He
Fig. 1. Effect of coating amount on removal efficiency and flow rate.
et al., 2018). This was also supported by the results of the EDS analysis.
The broadening of diffraction peaks indicated the cubic fluorite struc-
ture of CeO2 (Kartsonakis et al., 2008). Compared with nano-CeO2, the
XRD patterns of CF-CeO2 had weaker diffraction intensities, which ver-
ified that the small amount of nano-CeO2 particles were loaded on the
ceramic filters.
3.3. Factorial analysis of CF-CeO2 performance
In practical application, the performance of CF-CeO2 could be af-
fected by aqueous conditions. The factors of influent arsenic concentra-
tion, pH, background electrolyte concentration and their interactions
were analyzed through a 23 factorial design to investigate their influ-
ence on the arsenic-removal performance of CF-CeO2. The final polyno-
mial equations in terms of coded factors for arsenic removal efficiency is
as follow:
Arsenic removal efficiency
¼ 91:95–5:24A−4:67B−1:87C−3:83AB−0:64AC−0:79BC−0:56ABC
ð3Þ
where A, B, and C represented the coded influent arsenic concentration,
pH, and background electrolyte concentration, respectively. The corre-
sponding numbers were the coefficients that matched with the effects
and interactions of factors.
The result of normal plot of residuals for arsenic removal efficiency
approximated a straight line (Fig. S2), which indicated that the residuals
conformed as random dispersion and normal distribution (Ponnusami
et al., 2007). According to the ANOVA results shown in Table S2, the
Model F-value of 197.65 and the P-value < 0.0001 implied the model
was significant. In this case, A, B, C, AB, AC, BC, ABC were significant fac-
tors, in which factors of A, B, C and AB with P-value < 0.0001 had higher
significance. The “Pred R-Squared” of 0.9770 was in reasonable agree-
ment with the “Adj R-Squared” of 0.9892 and the ratio of 39.135 indi-
cated an adequate signal. As shown in Table S3, all factors had
negative effects on filtration performance. The influent arsenic concen-
tration had the largest effect and contributed 39.72% to the arsenic re-
moval performance. The effects of pH and background electrolyte
concentration had negative effects of −9.33 with a contribution of
31.50% and − 3.75 with a contribution of 5.07%, respectively. The inter-
active effect of AB was considerable with a contribution of 21.18%. The
interactive effects of AC and BC were − 1.29 with a contribution of
0.60% and − 1.58 with a contribution of 0.91%, respectively. As shown
in the pareto chart (Fig. S3), the effects were arranged in descending
order of the column length to indicate their significant levels. The results
 X. Yang et al. / Science of the Total Environment 750 (2021) 141510 5

Fig. 2. SEM image and EDX spectrum of CF-CeO2: (A) the surface of ceramic filter without nano-CeO2, (B) the surface of CF-CeO2, (C) interior cross section of CF-CeO2, (D) exterior cross
section of CF-CeO2.

confirmed that influent arsenic concentration, pH and the interactions
of these two factors had significant effects on the purification process.
The main effects and their interactions for factorial design on arsenic
removal efficiency are shown in Fig. 4. It was observed that the effect of
the variation of influent arsenic concentration and pH on arsenic re-
moval efficiency was greater than background electrolyte concentra-
tion. The increase of arsenic concentration in influent led to a
considerable decrease in the removal of arsenic. This was due to the
fact that the active adsorption sites were adequate for relatively few
adsorbed species at the low pollutant concentration (Tiwari et al.,
2007). Furthermore, at higher arsenic concentrations, there was a driv-
ing force to overcome the mass transfer barrier between the aqueous
phase and solid interface (Lalhmunsiama et al., 2014). The results fur-
ther suggested that the CF-CeO2 could remove As(V) effectively even
at much high concentration of As(V) in contaminated water. With the
increase of arsenic concentration, the slope on arsenic removal effi-
ciency at pH 9 was greater than that at 6. This indicated that the process
of removing arsenic was more sensitive to the variation of arsenic con-
centration in the alkaline environment. By contrast, with the increase of
arsenic concentration, the trends of arsenic removal efficiency were
very similar when the background electrolyte concentration was 0.001
and 0.100 mol/L. With the increase of pH values, the trends of arsenic re-
moval efficiency with background electrolyte concentration at high and
low levels were still similar. In the case of low arsenic concentration in
influent or acidic aqueous solution, even the background electrolyte
concentration was very high, CF-CeO2 could maintain good perfor-
mance on arsenic removal from water. It was observed that the interac-
tion of arsenic concentration and background electrolyte concentration
6 X. Yang et al. / Science of the Total Environment 750 (2021) 141510
Fig. 3. XRD spectra of CF, CeO2, and CF-CeO2.
was similar with the trend of influent arsenic concentration in terms of
main effect. Such pattern was also found in the interaction between pH
and background electrolyte concentration. This could be explained that
the impact of background electrolyte concentration could cause less in-
fluence on arsenic removal efficiency. However, under the same trend,
the increase of background electrolyte concentration could result in
the reduction of the arsenic removal efficiency to some extent. Thus,
both influent arsenic concentration and pH played important roles in ar-
senic removal.
3.4. Effects of different aqueous conditions
3.4.1. Effect of solution pH on As(V) removal
The macroscopic experiments were carried out to evaluate the effect
of solution pH on the removal of As(V). The removal efficiency of As
(V) by CF-CeO2 is depicted in Fig. 5A at different solution pH levels. It
was found that CF-CeO2 could remove arsenic with high efficiency
under low and moderate pH levels. In acidic solutions, the removal effi-
ciency changed slightly from 97.23% to 96.62% with elevated pH values.
Although a substantial decline was observed under alkaline conditions,
the removal efficiency remained above 80.00%. The ligand exchange
might play a dominant role in arsenic removal. Furthermore, the de-
crease in removal efficiency suggested that As(V) was removed through
not only ligand exchange but also coulomb forces (Chen et al., 2013).
These viewpoints are also supported by the following investigation
into the effect of background electrolyte concentration. As shown in
Fig. 5B, the zero point of Zeta potential of CF-CeO2 was about 7.1. The
As(V) in solution existed in negative ionic forms (HAsO2− 4 and
H2AsO− 4 ) in the pH range of 3–11. When the pH value was below 7.1,
the surface of CF-CeO2 carried positive charges, which facilitated the
electrostatic attraction between positive surface and arsenate anions.
When the pH value was above 7.1, the surface of CF-CeO2 and arsenic
species were both negatively charged, and a strong repulsive force led
to the rapid decline of the As(V) removal efficiency.
3.4.2. Effect of background electrolyte concentration on As(V) removal
As ions are abundant in natural waters, the influence of background
electrolyte concentration on As(V) removal was studied. The investiga-
tion into background electrolyte concentration could be used to distin-
guish the specific and nonspecific adsorptions of the anion (Zhao
et al., 2019). The impact of background electrolyte concentration on
the process of As(V) removal through CF-CeO2 is presented in Fig. 5C.
It was noted that with the increase of background electrolyte concentra-
tion up to 100 times (from 0.001 mol/L to 0.100 mol/L), the decrease in
corresponding As(V) removal efficiency was negligible, less than 10%.
Even though the ionic strength was at 0.100 mol/L, there was a very
minor impact on the removal of As(V). Previous studies pointed out
that the nonspecific adsorption was influenced dramatically with the
variation of background electrolyte concentrations. That could be attrib-
uted to the competitive adsorption between the background electrolyte
ions and adsorbed ions, whereas the specific adsorption was insensitive
to the change of ionic strength (Lee et al., 2015). Therefore, the removal
of As(V) by CF-CeO2 was predominant through the strong chemical
bond formation. A small reduction in removal efficiency could be expli-
cable with the fact that the weak force such as electrostatic attraction
also took part in the removal process. The results clearly showed that
the driving force of As(V) removal by CF-CeO2 was mainly through spe-
cific adsorption and followed by electrostatic attraction. This possible
mechanism would be further explored based on the characterization
analysis of FTIR, XPS and SR-XRF.
3.5. Simultaneous removal of As(V) and turbidity
Considering the complexity of components in natural water, the
common coexistence of various pollutants may affect the process of ar-
senic removal. Thus, the performance of CF-CeO2 to simultaneously re-
move arsenic and other component were evaluated. Simultaneous
removal experiments were conducted to explore the mutual influence
of turbidity and arsenic, since turbidity was the most typical index for
water quality evaluation. The result of turbidity removal without arse-
nic is shown in Fig. S4 as a reference for comparison. The results of si-
multaneous removal for turbidity and As(V) by CF-CeO2 are shown in
Fig. 6A and B, respectively. It was shown that arsenic contamination
had little effect on the performance of CF-CeO2 for turbidity removal.
The CF-CeO2 had great performances on turbidity removal (96.36%–
99.33%) from influents, no matter containing As(V) or not. With low
to medium levels of turbidity (0–100 NTU) in influent, the residual tur-
bidity in effluent was below the safe level (1 NTU) recommended by
WHO. Even at high turbidity levels (>100 NTU), the residual turbidities
were still below the WHO limit (5 NTU). The turbidity index of CF-CeO2
treated water can meet the standard of drinking water.
In comparison, turbidity level had significant effects on the perfor-
mance of CF-CeO2 for arsenic removal. Fig. 6B shows that the arsenic re-
moval efficiency increased significantly from 84.58% to 94.27% with the
increase of turbidity from 0 to 80 NTU in influent. With further increase
of turbidity to 180 NTU, the arsenic removal efficiency decreased by
16.59%. This could be attributed that the increase of turbidity indicated
the rise of kaolin concentration in solution. It was reported that kaolin
had some but limited ability to adsorb arsenic as clay sorbents
(Doušová et al., 2011; Uddin, 2017). Thus, kaolin with relatively low
concentration was involved to help arsenic removal to some extent.
However, as the kaolin concentration increased, CF-CeO2 surface could
be covered with a kaolin layer due to the attachment and accumulation
of kaolin during the filtration process, which blocked the contact be-
tween the CF-CeO2 and arsenic species. In addition, the presence of
background ions facilitated the agglomeration of kaolin, leading to the
decrease in available sites for arsenic adsorption (Huang et al., 1999).
The adsorption capacity of kaolin could not compensate for the loss of
active adsorption sites of CF-CeO2, which brought about the reduction
of arsenic removal efficiency. These results suggested that a medium
or low level of turbidity in aqueous environment favored the removal
of arsenic, while the excessive turbidity in aqueous environment
inhibited the removal of arsenic.
3.6. Mechanism for the removal of arsenic through CF-CeO2
During the filtration process, the influent contacted with the nano-
CeO2 coating and then went through the porous ceramic filter during
 X. Yang et al. / Science of the Total Environment 750 (2021) 141510 7

Fig. 4. Main and interaction effects plots on arsenic removal efficiency.

which arsenic was removed. In order to explore the mechanism of As The FTIR spectra of ceramics before and after filtration are shown in
(V) removal by CF-CeO2, FTIR, XPS, and SR-XRF studies were conducted Fig. 7A. The spectra illustrated that there was almost no change in terms
to analyze the roles of nano-CeO2 coating and the ceramic filter itself in of peak shift, new peak generation, and peak intensity occurred after fil-
arsenic removal. tration. It could be speculated that the ceramic adsorbed As(V) mainly

Fig. 5. (A) Effect of solution pH on the removal of As(V), (B) Zeta potentials of CF-CeO2, (C) Effect of background electrolyte concentration on the removal of As(V).
8 X. Yang et al. / Science of the Total Environment 750 (2021) 141510

in Table S4. The arsenic contents were increased from 0.00% to 0.51%
after the adsorption, which indicated that the ceramic also took part
in the arsenic removal. The atomic ratios of C, O, Ce, and As in the
nano-CeO2 coating before and after filtration are listed in Table S5. The
atomic ratio of As increased from 0.00% to 1.50% after adsorption, dem-
onstrating that the nano-CeO2 coating had a higher capacity to adsorb
arsenic compared to the ceramic. The states of arsenic and cerium on
nano-CeO2 coatings were further investigated through high-resolution
XPS spectra analyses. XPS core level spectra of Ce 3d (Fig. S5A) are com-
posed of three pairs of spin-orbital doublets which are related to the Ce
3d5/2 and Ce 3d3/2, since cerium element exists in Ce(III) and Ce(IV)
(Zhang et al., 2005). After As(V) adsorption, the valence state of Ce
had no change and the As 3d peak was at 45.2 eV (Fig. S5B), demonstrat-
ing no redox reaction occurred in the adsorption process. The XPS core
level spectra of O 1 s, C 1 s, Al 2p and Si 2p of ceramics shown in Fig. S6
did not change obviously after As(V) adsorption. This result was consis-
tent with the results of FTIR, which As(V) was removed by the ceramic
mainly through electrostatic attraction.
Fig. 8 also shows the XPS core level spectra of C 1 s and O 1 s from
nano-CeO2 coatings. The peak at about 288.5 eV in the spectrum of C

Fig. 6. Simultaneous removal of (A) turbidity, and (B) As(V) by CF-CeO2.

through electrostatic attraction. Fig. 7B presents the FTIR spectra of

nano-CeO2 coatings before and after As(V) adsorption. The wide band
at 3350 cm−1 can be assigned to the O\\H stretching vibration, and
the band at 1620 cm−1 is related to the bending vibration of water mol-
ecules, indicating the presence of water adsorbed on the surfaces and
interlayers of the CeO2 NPs (Nath et al., 2016; Xu et al., 2013). The
FTIR spectrum of pristine coating has a band at 1320 cm−1, which indi-
cated the vibration of carbonate species due to air exposure; another
band at 1060 cm−1 was corresponding to bending vibrations of hy-
droxyl groups on CeO2 NPs (Yu et al., 2015c). After As(V) adsorption,
these two peaks shifted to 1340 cm−1 and 1090 cm−1, respectively,
and the corresponding peak intensities decreased remarkably. This im-
plied that hydroxyl groups and carbonate groups on nano-CeO2 coating
played important roles in arsenic adsorption via the ligand exchange
(Wen et al., 2017; Zhang et al., 2005), although the As\\O band at
about 800 cm−1 was not clear due to the overlapping of extensive
peaks in this range (Li et al., 2010).
To further study the arsenic removal mechanism, XPS study was
used to analyze chemical compositions and functional groups of CF-
CeO2 before and after filtration. The XPS survey spectra of nano-CeO2
coatings and ceramics are shown in Fig. 8(A)-(B). It confirmed that
the arsenic had been adsorbed successfully onto the coating with the
appearance of As 3d peaks after filtration (Fig. 8A). In addition, no char-
acteristic peak of cerium appeared in the survey spectra of ceramics,
demonstrating that most of CeO2 NPs only stayed on the surface of CF-
CeO2 both before and after filtration (Fig. 8B). The atomic ratios of Al,
Si, C, O, Fe, and As in the ceramics before and after filtration are listed Fig. 7. FTIR spectra of (A) ceramics, and (B) nano-CeO2 coatings before and after filtration.
 X. Yang et al. / Science of the Total Environment 750 (2021) 141510 9

1 s (Fig. 8C) was assigned to CO2− 3 (Cao et al., 2012). After filtration
(Fig. 8D), the peak was shifted to 289.2 eV due to the presence of Na+
in the treated water, resulting in the formation of Na2CO3 (Stępniowski
et al., 2020). The contents of carbonate groups decreased from 22.40%
to 18.46% after adsorption, supporting that carbonate groups were in-
volved in ligand exchange. The O 1 s spectra in Fig. 8E consisted of
three peaks which were corresponding to metal‑oxygen bond (Ce\\O),
metal-hydroxyl groups (Ce-OH), and water molecular adsorbed on
CeO2 surface (Wen et al., 2018). After As(V) adsorption (Fig. 8F), a new
peak was observed, which was identified to be arsenic‑oxygen bond
(As\\O) with binding energy at 533.1 eV (Yu et al., 2015a; Yu et al.,
2017)., further verifying the successful adsorption of arsenic. Meanwhile,
the relative peak area ratio of Ce-OH groups obviously decreased from
45.00% to 22.19%, which also suggested that the replacement of these
groups by arsenic species occurred during the adsorption process. It
could be concluded that the presence of the abundant M-OH groups on
the coating surface might be the reason why the filters had a wonderful
capability to remove arsenic.
To investigate the stability of CF-CeO2, as well as further support the
study of arsenic removal mechanism, the SR-XRF mappings and spectra
of Ce and As concentration distributions on cross sections of CF-CeO2
were measured by SR-XRF. Synchrotron-based x-ray analysis can pro-
vide a high level of complementary elemental information for CF-CeO2
(Chen et al., 2019a; Chen et al., 2019b; Shen et al., 2020). In all SR-XRF
mappings of Fig. 9, the vertical position from top to bottom represents
the cross section from the surface of ceramic filter samples to the inter-
nal. As shown in the SR-XRF mapping of Ce on clean CF-CeO2 cross sec-
tion (Fig. 9A), the nano-CeO2 NPs were basically concentrated on the
surface of CF-CeO2. According to the SR-XRF spectrum (Fig. 9B), the
main components on CF-CeO2 surface are Ce and Fe. Meanwhile,

Fig. 8. XPS survey spectra of (A) nano-CeO2 coatings (the inset image shows the As 3d spectrum of used coating), and (B) ceramics before and after As(V) adsorption; C 1 s spectra of
(C) clean coating, and (D) used coating; O 1 s spectra of (E) clean coating, and (F) used coating.
10 X. Yang et al. / Science of the Total Environment 750 (2021) 141510

Fig. 9. The SR-XRF mappings and spectra of Ce and As concentration distribution on (A-D) clean CF-CeO2, (E-H) used CF-CeO2, and (I-L) used ceramic filters cross section.

Fig. 9C shows the SR-XRF spectrum from the inside part of CF-CeO2, in
which only characteristic peaks of Fe can be observed, but no character-
istic peak of Ce. This suggested that the observed Fe was from the ce-
ramic filter itself, since the clay used to make ceramic filter commonly
contained a certain amount of Fe, which has been displayed by EDS
results. The SR-XRF mapping of Ce on the used CF-CeO2 is shown in
Fig. 9E. After filtration, the strong signal area was still on the surface of
CF-CeO2. By contrast, the characteristic peaks of Ce did not appear in
the SR-XRF spectrum from the inside part (Fig. 9G). These results dem-
onstrated that there was almost no infiltration of nano-CeO2 from the
 X. Yang et al. / Science of the Total Environment 750 (2021) 141510
Fig. 10. Schematic diagram of the removal mechanism.
coating. Thus, it could be concluded that the nano-CeO2 coating was
steady on the surface of ceramic filter and did not migrate into the inter-
nal structure after CF-CeO2 was applied to the filtration.
As a reference for comparison, the unused CF-CeO2 did not contained
As, which was demonstrated by the SR-XRF mapping (Fig. 9D) and SR-
XRF spectra (Fig. 9(B)-(C)). After filtration, the signals of As were mainly
distributed on the surface of used CF-CeO2 (Fig. 9H), which was consis-
tent with the Ce distribution shown in Fig. 9E. According to the SR-XRF
spectrum (Fig. 9F), the characteristic peaks of both Ce and As had the
strongest intensities on the surface of used CF-CeO2. Besides, the XRF
spectrum from the inside part of used CF-CeO2 (Fig. 9G) did not contain
the characteristic peak of As. These implied that the adsorption of As
mainly happened on the CF-CeO2 surface due to the nano-CeO2 coating,
which was in accordance with previous experimental results in Fig. 8.
Thus, it further confirmed that almost all the arsenic could be removed
by the nano-CeO2 coating, and the arsenic contamination was success-
fully stuck on the surface of filter. The results of Ce and As distributions
on the used ceramic filter without nano-CeO2 coating also support the
above findings. Fig. 9I shows that there is almost no signal of Ce, demon-
strating that the ceramic filter itself did not contain Ce. The SR-XRF spec-
tra (Fig. 9(J)-(K)) also proved this point. The SR-XRF mapping of As in
Fig. 9L shows that the signals of As are distributed both on the surface
and interior of the ceramic filter. Compared the XRF spectrum from
the surface (Fig. 9J) and the inside part (Fig. 9K), the characteristic
peak intensity of arsenic in Fig. 9J is stronger than that in Fig. 9K, sug-
gesting that more arsenic was adsorbed on the surface of ceramic filter.
In the filtration process, the surface of ceramic filter was exposed to raw
water for a longer time, while the inside part of ceramic filter only
contacted with raw water through water flows, thus leading to more ar-
senic adsorbed on the surface. The above data revealed that the ceramic
filter itself was capable to adsorb As to a certain extent, but the capacity
was far from the nano-CeO2 coating, resulting in part of the arsenic
flowing down with the water and trapped by the interior ceramic. Nev-
ertheless, the arsenic removal ability of the ceramic filter itself further
ensured removal effectiveness and effluent quality of CF-CeO2.
Based on the FTIR, XPS, and SR-XRF analysis, the removal mecha-
nism of As(V) through CF-CeO2 is displayed in Fig. 10. For the nano-
CeO2 coating, the arsenic adsorption was mainly controlled by the
11
surface hydroxyl groups and carbonate groups through the ion-
exchange with arsenic species. Meanwhile, it was also affected by elec-
trostatic attraction to some extent. For the ceramic, the removal of arse-
nic mostly depended on the electrostatic adsorption. Thus, the removal
of As(V) by the CF-CeO2 had an integrated mechanism through the ion-
exchange and the participation of electrostatic attraction.
4. Conclusions
The exceptional performance of CF-CeO2 in the removal of As
(V) was demonstrated in this study. The properties of CF-CeO2 were de-
termined by the coating amount. Based on the consideration of both re-
moval efficiency and flow rate, the suitable coating amount of CeO2 was
determined for the production of CF-CeO2. The chemical properties of
aqueous solution such as influent arsenic concentration, pH and back-
ground electrolyte concentration had an influence on the effectiveness
of CF-CeO2. Based on the factorial analysis, influent arsenic concentra-
tion and pH were found to be the significant factors for influencing arse-
nic removal efficiency. Moreover, CF-CeO2 exhibited a good removal
capability over a wide pH range. In the treatment of natural water, the
existence of medium and low turbidity levels facilitated the removal
of arsenic, while the high turbidity level exhibited the opposite effect.
The macroscopic experiments regarding the effect of solution pH and
background electrolyte concentration and the microscopic characteriza-
tion with FTIR, XPS and SR-XRF suggested that the As(V) removal mech-
anisms mainly included ion-exchange and electrostatic attraction. The
findings in this study provide convincing evidence for the use of CF-
CeO2 as a potentially efficient and cost-effective approach of arsenic
groundwater decontamination. These results can help develop water
purification technology to improve drinking water safety in remote
areas. This ceramic filter can be transferred into a pot purifier with a
larger capacity to provide a point-of-use water-treatment device that
can satisfy the needs of household using in developing regions.
CRediT authorship contribution statement
Xiaohan Yang: Conceptualization, Investigation, Formal analysis,
Writing - original draft. Guohe Huang: Conceptualization, Formal
12 X. Yang et al. / Science of the Total Environment 750 (2021) 141510
analysis, Investigation. Chunjiang An: Conceptualization, Formal analy-
sis, Writing - review & editing. Xiujuan Chen: Conceptualization,
Writing - review & editing. Jian Shen: Writing - review & editing. Jianan
Yin: Writing - review & editing. Pei Song: Writing - review & editing.
Ziqing Xu: Writing - review & editing. Yongping Li: Writing - review
& editing.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgments
This research was supported by the National Key Research and
Development Plan (2016YFC0502800), the Natural Sciences Foundation
(51520105013, 51679087), and the Natural Science and Engineering
Research Council of Canada. The authors are particularly thankful to
the beamline of Very Sensitive Elemental and Structural Probe
Employing Radiation from a Synchrotron (VESPERS) at Canadian Light
Source for providing support in sample analysis. The authors are also
grateful to the comments and suggestions from the editor and the anon-
ymous reviewers.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.scitotenv.2020.141510.
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