Sustainability 14 08757

sustainability
Article
Occurrence, Comparison and Priority Identification of
Antibiotics in Surface Water and Sediment in Urbanized River:
A Case Study of Suzhou Creek in Shanghai
Xuhui Li, Yuan Yuan, Dou Zhang, Xiao Li, Dehuan Li and Xiangrong Wang *
Department of Environmental Science and Engineering, Fudan University, Shanghai 200438, China;
19210740046@fudan.edu.cn (X.L.); 20110740019@fudan.edu.cn (Y.Y.); 19110740011@fudan.edu.cn (D.Z.);
21110740033@m.fudan.edu.cn (X.L.); 18210740007@fudan.edu.cn (D.L.)
* Correspondence: xrxrwang@fudan.edu.cn; Tel.: +86-21-3124-8988
Abstract: Antibiotics in water have attracted increasing attention due to their potential threat to
aquatic ecosystems and public health. Most previous studies have focused on heavily polluted
environments, while ignoring urbanized rivers with high population density. Taking Suzhou Creek
in Shanghai as an example, this study attempted to explore the antibiotic pollution characteristics of
typical urbanized rivers. Further, it screened out priority antibiotics so as to provide reference for
the regular monitoring of antibiotics in urban surface water in the study’s later stage. Four classes
of 27 antibiotics in surface water samples and sediment samples were detected and analyzed by
SPE-UPLC-MS/MS under both wet season and dry season. Results demonstrate that the total amount
of antibiotics detected reached 1936.9 ng/L and 337.3 ng/g in water samples and sediment samples,
respectively. Through Pearson correlation analysis, it can be shown that there is a very significant
correlation between a variety of antibiotics in water and sediment. The results of ecological risk
Citation: Li, X.; Yuan, Y.; Zhang, D.;
Li, X.; Li, D.; Wang, X. Occurrence,
assessment based on risk quotient (RQ) show that certain antibiotics presented high and medium
Comparison and Priority risk to the surrounding ecosystem. Finally, the priority antibiotics selected by optimized priority
Identification of Antibiotics in screening method were EM, SPD, CLR and RTM. Therefore, we have proven that the antibiotics being
Surface Water and Sediment in discharged in urbanized rivers show different types of antibiotics, while presenting a toxicological
Urbanized River: A Case Study of risk to certain species.
Suzhou Creek in Shanghai.
Sustainability 2022, 14, 8757. Keywords: urbanized rivers; antibiotic; environmental risk assessment; priority antibiotics
https://doi.org/10.3390/su14148757
Academic Editor: Antonio

Miguel Martínez-Graña
1. Introduction
Received: 1 June 2022
Antibiotics are widely used by humans in their daily lives, as well as in crops and ani-
Accepted: 16 July 2022
mal medicine to treat diseases and promote growth [1]. Between 2000 and 2015, Antibiotic
Published: 18 July 2022
consumption, expressed in defined daily doses (DDD), increased 65% in 76 countries [2].
Publisher’s Note: MDPI stays neutral In 2013, the use of antibiotics in China was 162,000 tons, this figure is more than nine times
with regard to jurisdictional claims in that of the United States and more than 150 times that of the United Kingdom in the same
published maps and institutional affil- year [3]. Antibiotics cannot be completely absorbed or utilized by the receptor, 10–90%
iations.
of antibiotics may be excreted in the form of identical active compounds into the water
environment and sediments [4]. Antibiotics will be released into natural aquatic systems
in different ways, such as sewage treatment plant discharge, pharmaceutical wastewater
and domestic sewage [5,6]. Discharged antibiotics have chemical stability and bioaccumu-
Copyright: © 2022 by the authors.
lation ability, which can make them exist and accumulate in surface water and sediment
Licensee MDPI, Basel, Switzerland.
This article is an open access article
for a long time, and then pose significant risks to aquatic organisms, human health and
distributed under the terms and
ecological environments [7]. Studies have discussed the antibiotic residue level in coral reef
conditions of the Creative Commons fishes [8], vegetables [9] and drinking water [10]. Moreover, ARGs can also be horizontally
Attribution (CC BY) license (https:// transferred and amplified in the environment through genetic mechanisms under certain
creativecommons.org/licenses/by/ conditions [11].
4.0/).
Sustainability 2022, 14, 8757. https://doi.org/10.3390/su14148757 https://www.mdpi.com/journal/sustainability

Sustainability 2022, 14, 8757 2 of 19
Many studies have focused on the pollution characteristics of antibiotics around

the world [9,12–16]. China is the largest country in the production and consumption
of antibiotics, its emissions and potential risks have led to multiple studies in different
environmental zones in China, including reservoirs [17], aquaculture farms [18], oceans [19],
coastlines [20], lakes [21], upstream and downstream of sewage treatment plants [22],
rivers [23], sediments [24] and topsoil of first tier cities [25]. Previous studies have mostly
taken clearly polluted sewage receiving water bodies as their research objects to analyze
the occurrence and ecological risk of this pollution. However, there are few studies about
urbanized rivers, which are densely populated and ecologically fragile, while even fewer
people rank antibiotics in regard to the above areas. Rapid urbanization and population
increase mean more residents and more drug abuse, which leads to a lot of pollution of
urbanized rivers and brings more potential risks to the public [26,27]. Therefore, it is
necessary to study antibiotic pollution in urbanized rivers.
Suzhou Creek is 53 km long, and is located in the Yangtze River Delta (TRD). YRD
is an area with one of the most developed economies, the highest population density and
the most serious antibiotic pollution in China [28]. As a typical urbanized river, Suzhou
Creek connects Taihu Lake, Huangpu River and the East China Sea which has a developed
marine aquaculture. Its water environment not only affects aquatic organisms and radiated
residents, but also makes the greatest contribution to the antibiotic pollution of Huangpu
River [29]. The population density of Shanghai is about 3627 people/km2 while Suzhou
Creek passes through the downtown area. Therefore, extensive and intensive human
activities produce a large number of clinical antibiotics, which may dominate the antibiotic
pollution in Suzhou Creek, resulting in an extremely significant impact [24,30], and its water
pollution has become the main pressure affecting ecologically fragile coastal areas [31]. In
comparison with other regions, Suzhou Creek covers a smaller area with a considerably
larger population density. This provides an excellent opportunity to study the antibiotics
distribution in urbanized areas.
Water environments are the main source of antibiotic pollution [28]. However, most
previous studies have only detected the occurrence of antibiotics in surface water during
certain seasons. Due to poor sediment mobility and hypoxia, it is difficult for antibiotics
adsorbed on sediments to migrate further [32], while some antibiotics will desorb and enter
the water again, and some antibiotics will combine or decompose, synthesize maternal
antibiotics, and even produce more toxic products [33]. Therefore, simultaneously studying
the occurrence and ecological risk level of antibiotics in sediment and surface water in
different seasons has important theoretical significance for understanding the migration,
transformation, risk management and control of antibiotics in complex environments. The
detection requires efficient pre-treatment, precision instruments and professional analysis
technology. Moreover, quantifying antibiotics is very challenging, and not only takes a
long time, but also requires great expenses. Therefore, it is necessary to sort the antibiotics
detected in the environment and screen out the priority monitoring antibiotics. Existing
antibiotic priority screening methods either focus on the ecological risk [34,35], or their
steps are cumbersome and their methods difficult to implement [36]. The high requirements
for data sources and the incomplete consideration of indicators have led to the failure of
systematic and convenient antibiotic screening. Therefore, a simple and efficient screening
method is urgently needed.
Under both wet season and dry season, 27 typical antibiotics from four types of antibi-
otic were selected as target pollutants for sampling and analysis in this study according
to previous studies in Shanghai [10,37,38], and finally the concentration data of 14 an-
tibiotics were obtained through SPE-UPLC-MS/MS, including fluoroquinolones (QNs),
sulfonamides (SAs) and macrolides (MCs), which were the most widely used antibiotics in
China [39]. This study intends to solve three problems: (1) the occurrence status of antibi-
otics in surface water and sediment in Suzhou Creek under different seasons and compare
it with other study areas in the world; (2) the distribution of antibiotics in surface water
Sustainability 2022, 14, x FOR PEER REVIEW 3 of 20
and sediment and its ecological risk assessment; and (3) determination of the identifica-
tion priority antibiotics in Suzhou Creek using an optimized priority screening method.
and sediment and its ecological risk assessment; and (3) determination of the identification
priority antibiotics
2. Materials in Suzhou Creek using an optimized priority screening method.
and Methods
2.1.
2. Sample Collection
Materials and Methods
2.1. Sample
Surface Collection
water samples and sediment samples were collected in both May (wet sea-
son) Surface
in 2021 and
waterJanuary
samples (dry
andseason)
sedimentin 2022 at 21were
samples rivercollected
samplinginsites
both(P1–P21)
May (wet in season)
Shang-
hai, China, as Figure 1 shows. Both samples were collected at the same
in 2021 and January (dry season) in 2022 at 21 river sampling sites (P1–P21) in Shanghai, sampling site. The
selection
China, as of sampling
Figure sites Both
1 shows. mainly refers were
samples to previous
collected studies
at theinsame
Shanghai and site.
sampling the main
The
tributaries,
selection of at the samesites
sampling time, the sampling
mainly refers tosites are distributed
previous studies ininShanghai
the downstream of in-
and the main
dustrial land,
tributaries, at residential
the same time, areasthe
andsampling
agriculturalsitesland. The distanceinofthe
are distributed each sampling site
downstream of
varies from
industrial 1 km
land, to 5 km. areas
residential SuzhouandCreek passes through
agricultural land. The thedistance
city center, andsampling
of each the river
radiation
site variesarea
fromhas1 kma high
to 5 population
km. Suzhoudensity. The specific
Creek passes throughcoordinates of sampling
the city center, and thepoints
river
are shownarea
radiation in Supplementary
has a high populationTable S1. All water
density. The samples were collected
specific coordinates about 0.5points
of sampling m be-
lowshown
are the water surface with a Table
in Supplementary cylindrical
S1. Allsampler and stored
water samples wereincollected
a pre-cleaned
about brown glass
0.5 m below
bottle
the water(2.5surface
L) withwithscrew cap. Surface
a cylindrical waterand
sampler samples
storedwerein a stored at 4 °C.
pre-cleaned A grab
brown sampler
glass bottle
(2.5
wasL)usedwithtoscrew cap.
collect Surface water
sediment samples
samples, and polyethylene 4 ◦ C. Abags
were stored atplastic grabwere
sampler
usedwasto used
store
to collect sediment
sediment samples,
samples. Water and polyethylene
samples were transported plastic bagslaboratory
to the were used to store
with sediment
sediment sam-
samples. Water samples were transported to the laboratory with sediment
ples within 24 h for analysis. The concentrations of all detected antibiotics in surface water samples within
24 h for
were analysis.
in ng/L level,The
theconcentrations
concentrations of of all
all detected
detected antibiotics in sediment
surface waterwerewere in
in ng/g
ng/L
level. level, the concentrations of all detected antibiotics in sediment were in ng/g level.
Figure 1.
Figure 1. Locations
Locations of
of sampling
sampling sites
sites in
in Suzhou
Suzhou Creek.
Creek. P1 (Wetland
(Wetland Park),
Park), P2
P2 (Fishing
(Fishing center),
center), P3
P3
(Golf Club),
(Golf Club), P4
P4 (Wusong
(Wusong River
River Bridge),
Bridge), P5P5 (Shuangyang
(Shuangyang port),
port), P6
P6 (Huajiang
(Huajiang bridge),
bridge), P7
P7 (Tongpu
(Tongpu
road),P8
road), P8(Qilianshan
(Qilianshanbridge),
bridge),P9P9(Sightseeing
(Sightseeing dock),
dock), P10
P10 (Ludinglu
(Ludinglu bridge),
bridge), P11P11 (Gubeilu
(Gubeilu bridge),
bridge), P12
P12 (Kaixuanlu bridge), P13 (ECUPL), P14 (Wuninglu bridge), P15 (Zhenpinglu bridge), P16
(Kaixuanlu bridge), P13 (ECUPL), P14 (Wuninglu bridge), P15 (Zhenpinglu bridge), P16 (Changhualu
(Changhualu bridge), P17 (Changshoulu bridge), P18 (Guangfu road), P19 (North-south viaduct),
bridge), P17 (Changshoulu bridge), P18 (Guangfu road), P19 (North-south viaduct), P20 (Fujianlu
P20 (Fujianlu bridge), P21 (Garden Bridge).
bridge), P21 (Garden Bridge).
2.2. Chemicals
2.2. Chemicals and
and Reagents
Reagents
Twenty-seventypical
Twenty-seven typical antibiotics
antibiotics were
were screened,
screened, including
including 11
11 SAs
SAs (sulfamethoxazole
(sulfamethoxazole
(SMX), sulfisoxazole (SIZ), sulfadiazine (SDZ), sulfamerazine (SMR), sulfachloro-
(SMX), sulfisoxazole (SIZ), sulfadiazine (SDZ), sulfamerazine (SMR), sulfachloropyridazine
pyridazine (SCP), sulfathiazole (SAZ), trimethoprim (TMP), sulfapyridine (SPD),
(SCP), sulfathiazole (SAZ), trimethoprim (TMP), sulfapyridine (SPD), sulfamonomethoxine sulfa-
monomethoxine
(SMM), (SMM), sulfadimethoxypyrimidine
sulfadimethoxypyrimidine (SMM),(SMZ)),
(SMM), sulfamethazine sulfamethazine (SMZ)), 6
6 MCs (erythrocin
MCs (erythrocin
(EM), (EM),
roxithromycin roxithromycin
(RTM), (RTM),(CLR),
clarithromycin clarithromycin (CLR),(AZM),
azithromycin azithromycin
tylosin(AZM),
(TYL),
spiramycin (SPI)), 6 QNs (norfloxacin (NOR), enrofloxacin (ENR), ciprofloxacin (CIP),
difloxacin (DIF), pefloxacin (PEF), ofloxacin (OFL)), 4 TCs (oxytetracycline (OTC), chlorote-
tracycline (CTC), tetracycline (TC), and doxycycline (DOX)).
In the experiment, HPLC-grade acetonitrile was acquired from Thermofisher (Waltham,

MA, USA), LCMSMS-grade formic acid from Sigma-Aldrich (Shanghai, China), ultrapure
water from Millipore (Burlington, MA, USA), and the filler of solid phase extraction column
was copolymer of divinylbenzene and N-vinyl pyrrolidone (HLB, 500 mg/6 mL, Waters,
Milford, MA, USA).
2.3. Sample Pretreatment

Appropriate amounts of Na2 HPO4 , Na2 EDTA and citric acid were weighed to prepare,
respectively, 0.2 mol/L solution, mixed citric acid solution with Na2 HPO4 solution at 8:5
(V/V) to prepare McIlvaine solution, and then mixed McIlvaine and Na2 EDTA solution at
1:1 (V/V) to prepare 0.1 mol/L EDTA-McIlvaine extraction solution, which was adjusted to
pH 3.0 with H3 PO4 . For Acetonitrile, about 0.1% H3 PO4 was added and adjusted to pH
3.0. After freeze-drying, the sediment sample was ground through a 2 mm sieve, 1 g of
the ground sample was added to 10 mL EDTA-McIlvaine buffer, vortexed and mixed for
30 s, ultrasonic for 10 min, centrifugation at 12,000 R/min for 3 min. The supernatant was
transferred to another container for repeated extraction of the residue with organic mixed
extract. The extracts were combined, diluted with ultrapure water to 200 mL, and passed
through 0.5 mL 45 µm fiber filter membrane, adjusted to pH 3.0 with H3 PO4 .
The solid phase extraction column with 10 mL methanol and 10 mL ultrapure water
was activated to ensure the infiltration of the column head. The extract passed through a
solid phase extraction column under the action of natural gravity and was pumped dry by
vacuum pump. After the column was dried, the column was eluted with 10 mL 2% (volume
fraction) of ammonia and methanol at a flow rate of about 3 mL/min (about 1 drop/s).
The eluent was collected, blown via nitrogen in a 35 ◦ C water bath until nearly dry, the
volume fixed to 1 mL with acetonitrile/water (V/V = 10/90), ultrasonic or vortexed until
completely dissolved and passed through 0.22 µm organic filter membrane before being
transferred to brown 2 mL sample bottle for test. A blank test was conducted according to
the same operation method.
2.4. Analytical Methods

In this study, the target antibiotics were analyzed by ultra-high performance liquid
chromatography triple quadrupole mass spectrometry. The sample was on C18 column
(particle size 1.7 µm, with a column of 100 mm length and an inner diameter of 2.1 mm)
and was separated at a constant temperature of 40 ◦ C. The flow rate was 0.4 mL/min
and the injection volume was 10 µL. Mobile phase A was 5 mmol/L ammonium formate-
0.1% formic acid and mobile phase B is 5 mmol/L ammonium formate-0.1% formic acid
acetonitrile. The specific gradient elution conditions of liquid chromatography are recorded
in Supplementary Table S2 in the attachment.
Mass spectrometry includes electrospray ionization (ESI), capillary voltage of 2.5 KV,
ion source temperature of 150 ◦ C, desolvent temperature of 600 ◦ C, desolvent gas flow of
1000 L/h, cone hole gas flow of 50 L/h, collision gas of argon, desolvent gas of N2 , mobile
phase a of 5 mmol/L ammonium formate-0.1% formic acid acetonitrile, mobile phase B of
5 mmol/L ammonium formate-0.1% formic acid-water. The elution method was gradient
elution. 0.0–0.5 min, 5% A, 0.5–5 min, 5–20% A, 5–8 min, 20–90% A, 8–10 min, 90% A,
10–13 min, 5% A. Supplementary Table S3 shows specific monitoring ion pair information
and other information.
2.5. Quality Analysis and Control

An appropriate amount of standard was accurately weighed and put into a 1 mg/mL
standard solution with acetonitrile, in which quinolones were dissolved in acetonitrile and
a small amount of 0.1% formic acid water. The standard solutions were accurately absorbed
and diluted with acetonitrile into a 1 mg/L mixed standard solution, and then stored at
4 ◦ C. The mixed standard solutions were accurately absorbed and prepared with the initial
mobile phase, with concentrations of 0.005 µg/L, 0.01 µg/L, 0.05 µg/L, 0.1 µg/L, 0.5 µg/L,
1 µg/L, 5 µg/L, 10 µg/L series of standard solutions.
The prepared series of standard solutions were taken and determined for both the
quantitative ion peak area and concentration for linear regression analysis. During the
experiment, one laboratory blank and solvent blank were analyzed in every 10 samples
as controls, and the spiked recovery was determined. The target antibiotics in each blank
sample were lower than the detection limit. Analysis of field blank and procedure blank
showed that there was no pollution in the extraction and sampling process. Six samples with
different concentrations were prepared after adding standard solution. After pretreatment,
the recovery and relative standard deviation (RSD) of six parallel determinations were
calculated. The results show that the relative standard deviation ranged from 0.672% to
15.5%, and the recovery ranged from 56.2% to 128.0%.
2.6. Pseudo Distribution Coefficient

The resistance genes may be influenced by antibiotics accumulated in sediment, so it
is very important to quantify the distribution behavior of antibiotics between water and
sediment. Although there is no balance between the content of antibiotics in water and
sediment in aquatic ecosystems, the pseudo distribution coefficient (Kd ) is still an important
index to indicate the distribution behavior of antibiotics affected by all environmental
factors in a water–sediment system. The Kd value is calculated according to the formula:
Kd = Cs /Cw , where Cs represents the antibiotic concentration in sediments, Cw represents
the antibiotic concentration in surface water.
2.7. Environmental Risk Assessment

Some antibiotics widely exist in the water environment of Shanghai [38] with different
levels of pollution. According to the European technical guidance document on risk
assessment, the environmental risk of antibiotics in aquatic environment was assessed
based on risk quotient [34,35,40]. In order to evaluate the environmental risk of antibiotics,
the following formula was used to calculate the risk quotient (RQ) for evaluation, including
the use of the data of freshwater algae (phototrophic level), Daphnia magna (invertebrates)
and fish (vertebrates).
RQ = MEC/PNEC (1)
PNEC = (EC50 or LC50 or NOEC)/AF (2)
where MEC is the measured environmental concentration and PNEC is the predicted no-
effect concentration. EC50 (LC50 ) is the median effective or lethal concentrations obtained
from the existing studies and ECOSAR database, and no observed effect concentration
(NOEC) represents chronic toxicity [41]. When more than one toxicity dataset is obtained
at the same nutritional level, the dataset with the strongest effect is used based on the
worst-case consideration. AF is the safety factor of acute toxicity and chronic toxicity,
which are 1000 and 100, respectively [42]. Generally, The RQ values were classified into
four risk levels, including insignificant risk(RQ < 0.01), low risk(0.01 < RQ < 0.1), median
risk(0.1 < RQ < 1), and high risk(RQ > 1) [43].
2.8. Priority Antibiotics Screening Method

In order to comprehensively determine the priority types of antibiotics to be monitored,
on the basis of the identification method which is easy to implement and combines the
occurrence of antibiotics with ecological risk [29,44], the screening conditions are added
and improved, including the following four conditions.
(1) High frequency of detection (>80%)
The high detection frequency indicates that the antibiotic is representative and uni-
versal in the whole study area with greater potential harm to aquatic organisms. High
frequency of detection was considered if levels were over 80%.
(2) Strong positive correlation with total antibiotic concentration (SUM) (p < 0.05) or high
concentration antibiotics
If there is a strong positive correlation between an antibiotic and sum, such antibiotic
will have a strong indication of the total antibiotic concentration. Pearson correlation
coefficient (R) between single antibiotic concentration and total antibiotic concentration
was calculated. Only a robust (r > 0.6) and statistically significant (p < 0.05) correlation will
be considered as strong correlation. The ratio of each antibiotic concentration to the total
antibiotic concentration was calculated, and then the average value was obtained. Antibiotic
with a proportion greater than the average is defined as high concentration antibiotic.
(3) Significant risk of acute or chronic toxicity to aquatic organisms (RQ > 0.01)
This restriction mainly considers the acute or chronic ecological risks to aquatic animals
and plants. When the RQ value is greater than or equal to 0.01, the antibiotic is selected,
which indicates that the antibiotic studied may cause potential adverse effects on aquatic
organisms in the short or long term. Antibiotics are considered to meet constraints as long
as they have acute or chronic ecological risks.
(4) Detection frequency is over 30% in sediment
This constraint is designed to give priority to the monitoring of antibiotics with certain
detection frequency in sediment. Any antibiotic with 30% detection frequency or more
would be selected. Adding this restriction allows us to take into account the enrichment of
antibiotics in the sediment environment, and then more accurately screen out antibiotics
with great potential pollution hazards.
Antibiotics meeting the above four constraints will be selected as priority antibiotics,
and regular monitoring is recommended.
3. Results and Discussion

3.1. Occurrence of Selected Antibiotics
3.1.1. Antibiotics in Surface Water
The histogram of target antibiotic concentration in surface water in each sampling
site of Suzhou Creek is shown in Figure 2. The detected antibiotics in study area belong to
SAs, QNs and MCs classes. The occurrence of various antibiotics in aquatic systems will be
affected by the chemical stability and distribution characteristics brought by their special
structure. SAs have high solubility and chemical stability in water [45], while MCs are
easy to be adsorbed by sediments [46]. QNs are easily photodegradable [47]. Tetracyclines
(TCs) are widely used to protect animal health, are added to animal feed at sub therapeutic
levels to prevent infection and act as growth promoters [48]. TCs are the most widely
used veterinary drugs and food additives in aquaculture and animal husbandry in China.
There is no large-scale aquaculture and animal husbandry in the center of Shanghai, so
this may be one of the reasons why relevant types of antibiotics are not detected in this
study. This also indicates that the main sewage types in the study area do not include
aquaculture wastewater. The concentration was relatively constant, meanwhile, there was
little difference in antibiotic composition and distribution at different sampling points.
The detection frequency of antibiotics in the study area is summarized in Table 1.
Twenty-seven antibiotics were under detection, 12 antibiotics with different detection rates
were detected in water samples. The total concentrations of antibiotics detected in surface
water in the two seasons were 425.2 ng/L and 1734.7 ng/L. The detection frequency of
antibiotics was 5–100%. SPD was the main antibiotic detected, and the detection rate was
100%. There was a large gap of concentration between SPD and other detected antibiotics,
followed by RTM, CLR and SMX. Similarly, the detection rate was also 100% in the sampling
area. The detection concentrations of OFL, TMP and SMM were the lowest, and the range
of the detection rate was 35–100%. The concentration of antibiotics detected in the dry
season was generally higher than in the wet season, and five kinds of antibiotics, such as
SDZ, SMR, SCP, EM and AZM, were detected, in which the concentration of EM was the
highest among all antibiotics.
AZM
CLR
120 RTM
16 EM
CLR
SMM
RTM
SPD
14 SMM 100
SPD
TMP
TMP SCP
concentration （ng/L）
12 SMX SMR
OFL 80 SDZ
SMX
concentration (ng/L)
10
60
8
6 40
4
20
2
0
0
P1
P2
P3
P4
P5
P6
P7
P8
P9
0
1
2
3
4
5
6
7
8
9
0
1
P1
P1
P1
P1
P1
P1
P1
P1
P1
P1
P2
P2
P1 P2 P3 P4 P5 P6 P7 P8 P9 P10 P11 P12 P13 P14 P15 P16 P17
dry season
wet season
(a) (b)
Figure
Figure2. 2.
Concentrations
Concentrations of of
thethe
antibiotics detected
antibiotics in in
detected thethe
surface water
surface watersamples
samplesfrom thethe
from 2121
sites in in
sites
Suzhou Creek: (a) detected antibiotics from each site in wet season; (b) detected antibiotics
Suzhou Creek: (a) detected antibiotics from each site in wet season; (b) detected antibiotics from each from
each
sitesite in dry
in dry season.
season. P1 (Wetland
P1 (Wetland Park),
Park), P2 (Fishing
P2 (Fishing center),
center), P3 (Golf
P3 (Golf Club),Club), P4 (Wusong
P4 (Wusong River
River Bridge),
Bridge), P5 (Shuangyang port), P6 (Huajiang bridge), P7 (Tongpu road), P8 (Qilianshan bridge), P9
P5 (Shuangyang port), P6 (Huajiang bridge), P7 (Tongpu road), P8 (Qilianshan bridge), P9 (Sight-
(Sightseeing dock), P10 (Ludinglu bridge), P11 (Gubeilu bridge), P12 (Kaixuanlu bridge), P13
seeing dock), P10 (Ludinglu bridge), P11 (Gubeilu bridge), P12 (Kaixuanlu bridge), P13 (ECUPL),
(ECUPL), P14 (Wuninglu bridge), P15 (Zhenpinglu bridge), P16 (Changhualu bridge), P17 (Chang-
P14 (Wuninglu
shoulu bridge), P18bridge),
(Guangfu P15road),
(Zhenpinglu bridge), P16
P19 (North-south (Changhualu
viaduct), bridge),
P20 (Fujianlu P17 P21
bridge), (Changshoulu
(Garden
bridge), P18 (Guangfu road), P19 (North-south viaduct), P20 (Fujianlu bridge), P21 (Garden Bridge).
Bridge).
The
Table Detection frequency
1. detection frequencyand
ofconcentration of the
antibiotics in antibiotics
study in surface
area water samples.
is summarized in Table 1.
Twenty-seven antibiotics were under detection, 12 antibiotics with different detection
Compounds rates Wet
wereSeason (ng/L)
detected Dry Season
in water samples. The total concentrations (ng/L)
of antibiotics detected in
Freq. surface water in the
Median two seasonsMax
Mean were 425.2 ng/L
Freq.and 1734.7 ng/L. The detection
Median Mean frequency
Max
OFL 82% of antibiotics
0.3 was 5–100%.
0.4 SPD was
0.4 the main antibiotic detected, and the detection rate
SMX 100% was 100%.
0.2 There was 0.2 a large gap
0.3of concentration
100% between 2.4SPD and other
2.4 detected2.9anti-
TMP 35% 0.1followed by
biotics, 0.1RTM, CLR 0.1 100%
and SMX. Similarly, 0.3
the detection rate 0.3
was also 100%0.4 in
SPD 100% 7.9
the sampling area. 8.4
The detection 10.4 100%of OFL, TMP
concentrations 21.8 and SMM 22.6 30.6
were the lowest,
SMM 82% 0.1 0.1 0.1 100% 0.5 0.5 0.6
and the range of the detection rate was 35–100%. The concentration of antibiotics detected
RTM 100% 1.7 1.7 2.1 100% 1.5 1.7 3.7
CLR 100% in the1.3
dry season was 1.3 generally higher
1.7 than in the wet season,
100% 1.1 and five kinds
1.2 of antibiotics,
2.3
SDZ such as SDZ, SMR, SCP, EM and AZM, were detected, in which
100% 0.5 the concentration
0.6 of0.9EM
SMR was the highest among all antibiotics. 5% 0 0 0.4
SCP 100% 0.4 0.4 0.6
EM 100%
Table 1. Detection frequency and concentration of antibiotics in 52.9 51.9
surface water samples. 69.5
AZM 71% 1.3 1.0 1.9
Wet Season (ng/L) Dry Season (ng/L)
Compounds
The heavy precipitation and the strong fluidity of the river in Median
Freq. Median Mean Max Freq. MeanwillMax
the wet season dilute
OFL
the antibiotics 82%
in the river, thus0.3
reducing 0.4 0.4 concentration there [49]. The high
the antibiotic
temperature
SMX and strong
100% light in0.2
May accelerated
0.2 the0.3
degradation
100% of antibiotics
2.4 in water
2.4 2.9[50].
Some antibiotics are
TMP concentrated
35% 0.1 in the sediments,
0.1 0.1and, 100%
because little
0.3 light 0.3
reaches0.4
these
sediments
SPD it is not easy
100% for photodegradation
7.9 8.4 to occur, resulting
10.4 100% in
21.8the accumulation
22.6 30.6 of
some antibiotics
SMM there
82%[18]. Finally,
0.1 the demand
0.1 for drugs
0.1 in winter
100% is generally
0.5 0.5higher
0.6than
in summer,
RTM which leads
100% to a higher
1.7 level of
1.7 antibiotic
2.1 pollution.
100% Among
1.5 them,
1.7 SMX3.7and
SPD, which are often used as clinical drugs, have higher concentrations in winter, and EM,
CLR 100% 1.3 1.3 1.7 100% 1.1 1.2 2.3
which is often used as a household drug, is detected in winter and shows extremely high
SDZ 100% 0.5 0.6 0.9
pollution concentrations. Therefore, compared with the dry season, the wet season has
SMR 5% 0 0 0.4
lower antibiotic concentration and fewer antibiotic species [51,52].
SCP 100% 0.4 0.4
Sulfonamide antibiotics and macrolide antibiotics were the most abundant antibiotics 0.6
EM 100% 52.9 51.9
in the detection results of surface water, accounting for 99.9% of the total antibiotic concen- 69.5
AZM
tration. SAs have high water solubility and chemical stability 71% [53], so
1.3these antibiotics
1.0 1.9 are
very easy to retain and diffuse in water. As shown in Figure 2, the largest concentration
of antibiotics detected in the surface water was SPD. SPD is mainly used to treat human
diseases and belongs to the SA class. SMX is one of the 14 SAs required to be tested
preferentially by the U.S. Food and Drug Administration. SMX has been widely detected
in many surface water environments in China [54]. TMP is a kind of SA synergist, which
is often used in combination with SA antibiotics to enhance their therapeutic effect. It
can be seen from this detection data that the concentration distribution trend of these two
antibiotics was consistent, so they were frequently detected in Suzhou Creek. TCs were not
detected in this study, maybe because of their strong chelating agent, their low solubility
and stability in water [55], and how prone they are to photodegradation [56]. Similarly, the
detection frequency and concentration of TCs were low according to previous studies on
Shanghai [29].
Quinolone antibiotics, which are easily photolyzed, are widely used in China because
of their affordable price and their lack of cross resistance with other drugs [57], OFL was the
only quinolone antibiotic detected in this study, with an average concentration of 0.32 ng/L.
It has been detected in many surface water environments, such as the rivers in Zhuhai [34],
where the concentration level was 2–3 orders of magnitude higher than the results of this
study. MCs are often used as clinical drugs and pet drugs, at the same time, they are the
third most dominant antibiotics in water [58]. In this study, four major macrolide antibiotics
RTM, CLR, AZM and EM were detected in surface water. These four antibiotics are widely
used all over the world. For example, CLR is one of the most commonly detected antibiotics
in some developed countries in Europe [59]. In this study, the detection concentration and
frequency of macrolide antibiotics are generally average, but are the lowest compared with
other study areas [54]. Among these, the detection concentration of EM was higher than
that of all other antibiotics, and its average value reached 51.9 ng/L. This is because this
kind of antibiotic is a typical representative of the same type of antibiotic, which is widely
used because of its easy availability, low price and wide application range.
3.1.2. Antibiotics in Sediment

Eight antibiotics were detected in sediment (Figure 3). The detection frequency of
antibiotics in sediment was 6–100% (Table 2). AZM had the highest detection concentration
in the two phases, and the detection rate was 100%. EM had a significantly increased
detection concentration in the dry season. There was a large gap between the two antibiotics
and other detection antibiotics. The concentrations of SPD, RTM and CLR were the second,
and these three antibiotics had very high detection frequency. The detection concentrations
of SMZ, STZ and SMX were the lowest, and the detection rate was between 6–47%. These
three kinds of antibiotics were not detected in the dry season. SAs and MCs were the
most abundant antibiotics in the results, accounting for 50% of the total antibiotics in
sediment samples respectively. Similar to the results of surface water samples, EM, SMX,
SPD, CLR and RTM in these two classes of antibiotics were also detected in sediments,
which indicate that these antibiotics were widely used in the study area. In this study, the
antibiotic pollution level in sediment did not change significantly with seasons, which was
different from the general pattern because the concentration distribution of antibiotics in
the sediment environment of urbanized rivers was not easily affected by seasonal changes.
At the same time, the sediment dredging project was carried out constantly in the study
area in dry season, which eventually led to the inconsistency between this study and the
general pattern.
MC, as an important type of clinical drug, has been reported to mainly exist as a cation
and adsorbed on solid particles owing to its high Kow [60,61]. It can eventually remain
stable in sediment [58], something which can explain their high detection frequency there
in sediment environments. On the contrary, SA showed a lower concentration due to its
strong hydrophilicity. AZM was the antibiotic with the largest concentration in sediment,
and AZM belongs to the same type of antibiotic as MCs. STZ and EM detected in sediment
belongs to antibiotics banned by China’s aquaculture industry in aquatic food and bait
animals. The commonly used antibiotics in aquaculture belong to TCs and QNs [62], and
these antibiotics have strong adsorption on sediments and particles [63]. These antibiotics
SMX, SPD, CLR and RTM in these two classes of antibiotics were also detected in sedi-
ments, which indicate that these antibiotics were widely used in the study area. In this
study, the antibiotic pollution level in sediment did not change significantly with seasons,
which was different from the general pattern because the concentration distribution of
antibiotics in the sediment environment of urbanized rivers was not easily affected by
seasonal changes. At the same time, the sediment dredging project was carried out con-
stantly in the study area in dry season, which eventually led to the inconsistency between
were
this not and
study detected in sediment
the general in the study area. It can be seen that the type of sewage
pattern.
source in the study area is very likely to exclude aquaculture wastewater.
AZM
CLR
RTM AZM
25 EM 10
CLR
SPD RTM
STZ EM
20 SMZ
concentration （ng/g）
8 SPD
concentration (ng/g)
SMX
15 6
10 4
5 2
0 0
P1 P2 P3 P4 P5 P6 P7 P8 P9 P10 P11 P12 P13 P14 P15 P16 P17 P18 P19 P20 P21
P1
P2
P3
P4
P5
P6
P7
P8
P9
0
1
2
3
4
5
6
7
P1
P1
P1
P1
P1
P1
P1
P1
dry season
wet season
(a) (b)
Figure
Figure3.3.Concentrations
Concentrationsofofthetheantibiotics
antibioticsdetected
detectedininthe
thesediment
sedimentsamples
samplesfrom
fromthethe2121sites
sitesinin
Suzhou Creek: (a) detected antibiotics from each site in wet season; (b) detected antibiotics
Suzhou Creek: (a) detected antibiotics from each site in wet season; (b) detected antibiotics from from
each
each site in dry season. P1 (Wetland Park), P2 (Fishing center), P3 (Golf Club), P4 (Wusong River
site in dry season. P1 (Wetland Park), P2 (Fishing center), P3 (Golf Club), P4 (Wusong River Bridge),
Bridge), P5 (Shuangyang port), P6 (Huajiang bridge), P7 (Tongpu road), P8 (Qilianshan bridge), P9
P5 (Shuangyang port), P6 (Huajiang bridge), P7 (Tongpu road), P8 (Qilianshan bridge), P9 (Sight-
(Sightseeing dock), P10 (Ludinglu bridge), P11 (Gubeilu bridge), P12 (Kaixuanlu bridge), P13
seeing dock),
(ECUPL), P10 (Ludinglu
P14 (Wuninglu bridge),
bridge), P11 (Gubeilubridge),
P15 (Zhenpinglu bridge),P16P12(Changhualu
(Kaixuanlu bridge), P13 (Chang-
bridge), P17 (ECUPL),
P14 (Wuninglu bridge), P15 (Zhenpinglu bridge), P16 (Changhualu bridge), P17
shoulu bridge), P18 (Guangfu road), P19 (North-south viaduct), P20 (Fujianlu bridge), P21 (Garden(Changshoulu
bridge), P18 (Guangfu road), P19 (North-south viaduct), P20 (Fujianlu bridge), P21 (Garden Bridge).
Bridge).
Table
Table2.2.Detection
Detectionfrequency
frequencyand
andconcentration
concentrationofofantibiotics
antibioticsininsediment
sedimentsamples.
samples.
Wet Season (ng/g) Wet Season (ng/g)

Compounds
Dry Season
Dry Season (ng/g) (ng/g)
Compounds Freq. Median Mean Max Freq. Median Mean Max
Freq. Median Mean Max Freq. Median Mean Max
EM 53% 0.1 0.1 0.3 86% 1.4 2.1 7.8
EM 53% 0.1 0.1 0.3 86% 1.4 2.1 7.8
RTM 100% RTM
0.4 100%0.5 0.4 1.7 0.5 1.7
95% 95% 0.3 0.3 0.50.5 1.4
1.4
CLR 100% CLR
0.5 100%0.5 0.5 1.7 0.5 1.7
95% 95% 0.3 0.3 0.50.5 1.9
1.9
AZM 100% AZM
9.7 100%9.8 9.7 19.9 9.8 19.9
100% 100%1.8 1.8 2.72.7 4.5
SPD 100% 1.4
SPD 100%1.8 1.4 4.7 1.8 38%
4.7 38% 0 0 0.10.1 0.5
0.5
SMX 47% 0 0.3 2.7
SMX 47% 0 0.3 2.7
SMZ 18% 0 0 0.2
STZ 6% SMZ
0 18% 0 0 0.3 0 0.2
STZ 6% 0 0 0.3
3.1.3. Comparison of Antibiotics in Different Studies
MC, as an important type of clinical drug, has been reported to mainly exist as a
cationFigure 4 and Table
and adsorbed S4 show
on solid the concentration
particles comparison
owing to its high of various
Kow [60,61]. selected antibi-
It can eventually re-
main stable in sediment [58], something which can explain their high detectionobtain
otics in some surface water environments at home and abroad. In order to more
frequency
comparative
there data,
in sediment this study selected
environments. On thethe data measured
contrary, SA showed in wet season
a lower for comparison.
concentration due
Specifically, 7 antibiotics including OFL, SMX, TMP, SPD, SMM, RTM and
to its strong hydrophilicity. AZM was the antibiotic with the largest concentration CLR were
in sed-in-
volved.
iment, The
and AZMother concentrations
belongs of type
to the same antibiotics were either
of antibiotic collected
as MCs. STZ and from
EMthe studiesinor
detected
calculated using the data provided in the studies (Supplementary Table S4). The concentra-
sediment belongs to antibiotics banned by China’s aquaculture industry in aquatic food
tions those studies reported as ‘not detected’ or ‘below detection limit’ were assigned not
and bait animals. The commonly used antibiotics in aquaculture belong to TCs and QNs
detected [64]. As an urbanized river, Suzhou Creek receives a smaller amount of sewerage
[62], and these antibiotics have strong adsorption on sediments and particles [63]. These
from husbandry and aquaculture, and there are relatively few pollution sources. More-
over, the water body of the river has large fluidity and a strong dilution effect. Therefore,
compared with other domestic rivers, lakes and other surface water bodies, the antibiotic
pollution concentration in Suzhou Creek is relatively low. Overall, the relatively different
concentration levels indicate that the frequency, quantity and treatment level of the same
drug are different in different regions.
erage from husbandry and aquaculture, and there are relatively few pollution sources.
Moreover, the water body of the river has large fluidity and a strong dilution effect. There-
fore, compared with other domestic rivers, lakes and other surface water bodies, the anti-
biotic pollution concentration in Suzhou Creek is relatively low. Overall, the relatively
different concentration levels indicate that the frequency, quantity and treatment level of
Sustainability 2022, 14, 8757 the same drug are different in different regions. 10 of 19
100 100
80 80
CLR
CLR
Percantage (%)
Percantage (%)
RTM RTM
60 60 SMX
SMX
SMM SMM
TMP TMP
SPD SPD
40 40
OFL OFL
20 20
0 0
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34
China Abroad
(a) (b)
Figure
Figure4. 4.
Comparison
Comparisonof target antibiotics
of target concentrations
antibiotics in surface
concentrations waterwater
in surface in different regions:
in different (a)
regions:
comparison with with
(a) comparison domestic research;
domestic (b) comparison
research; with with
(b) comparison abroad research.
abroad research.
Antibiotic
Antibiotic abuse
abuse is ismost
mostcommon
commoninindeveloping
developingcountries,
countries,suchsuchasasisakavagu
isakavagunakka- nakkav-
vagu
aguin inIndia
India[65],
[65],which
whichisislocated
locatedininHyderabad,
Hyderabad,one oneofofthe theworld’s
world’slargest
largesthubshubs forfor
the
the
bulk
bulk drug
drug industry.
industry. OFL OFLconcentration
concentration detected in this
detected in river reaches
this river 10,00010,000
reaches ng/L. The
ng/L. BTHThe
region
BTH is the capital
region economic
is the capital circle ofcircle
economic China,of with
China, a large
with population density density
a large population and rapid and
rapid economic
economic development.development.
OFL with OFLa with a concentration
concentration of 11,735 of 11,735
ng/L ng/L was measured
was measured in
in Wangyang
Wangyang River River in this
in this region
region [62].[62].
TheThePRD PRD is the
is the largest
largest urban
urban agglomeration
agglomeration with
with
population
population andand area
area in in
thethe world.
world. Quite
Quite highhigh concentrations
concentrations of OFL
of OFL werewerealso also
detecteddetected
in
in Hong
Hong KongKong [66] Pearl
[66] and and Pearl
RiverRiver
[34], [34], the antibiotic
the antibiotic concentrations
concentrations in both
in both regions
regions werewere3–
3–4 orders
4 orders of magnitude
of magnitude higherhigher than those
than those in thisin this study.
study. Compared Compared
with thewith the Huangpu
Huangpu River
in Shanghai [38] which also belongs to the YRD, the detected concentration of OFL inOFL
River in Shanghai [38] which also belongs to the YRD, the detected concentration of thisin
this study was low and one order of magnitude less than
study was low and one order of magnitude less than that in Huangpu River [22]. that in Huangpu River [22].
Compared
Compared with
with other
other river
river basins
basins inin China,
China, thethe concentrations
concentrations ofofSASA and
and MC MC inin the
the
study
study areawere
area weregenerally
generally1–2 1–2orders
ordersofofmagnitude
magnitudeless, less,andandthethepollution
pollution level
level was
was simi-
similar
lartotothat
thatofof
manymany rivers
riversin Japan [67].[67].
in Japan SMM SMMwaswasdetected
detectedonly only
in some areas areas
in some [68]. The
[68].concen-
The
trations of SMX, SPD and SMM in the study area were low
concentrations of SMX, SPD and SMM in the study area were low in general, similar to in general, similar to the Yellow
theRiver
Yellow [69], Barigui
River [69],River
Barigui[13] and[13]
River La Poudre River [70].
and La Poudre River Barigui River, River,
[70]. Barigui which which
is located
is
in Curitiba, one of the most developed and populous cities
located in Curitiba, one of the most developed and populous cities in Brazil, has similarin Brazil, has similar charac-
teristics withwith
characteristics the study area. area.
the study SMXSMX has the
hashighest detection
the highest rate ofrate
detection all of
theall
above surface
the above
water areas, and is selected as the representative antibiotic of spatial variation of antibiotics
in China [28]. Haihe River [71] and Wangyang River [62] located in the above densely
populated region BTH have detected high concentrations of SMX. Antibiotic resistance
can be produced when antibiotics reach a concentration of 100 ng/L, while the antibiotic
concentration detected in the above rivers is as high as 1000 ng/L. Charmoise River belongs
to the Seine River basin, which is characterized by a high population density within the
Paris conurbation and the basin itself receives large amounts of domestic effluents [72]. The
Nairobi river basin in Kenya [73] and the rivers of Durban in South Africa [74] are both
located in informal settlements that are characterized by overcrowding and poor sanitation,
moreover, the former is exposed to diseases such as HIV/AIDS. The rivers of Kumasi lie
in Ghana [9], a low and middle-income country where the public has easy and multiple
access to antibiotics. SMX has been detected in all the mentioned watersheds with high
concentrations of 1435 ng/L, 13765 ng/L, 2561 ng/L and 2861 ng/L, respectively. TMP is
often used with SMX, so it has a relatively high detection rate. TMP with concentrations
above 1000 ng/L was detected in Wangyang River [62], Ravi River [75] and Kenya [73].
RTM is one of the most concerning antibiotics [28]. The average concentration of RTM
in this study is much lower than that in German [76] and Australian rivers [77], and the
concentration range is equivalent to that in Chenhu Lake [78] and Songhua River [79].
The detected concentration of CLR in other watersheds is low, basically at the level of
1–10 ng/L, such as the Jialing River in Chongqing [54] and the Chester River in the United
States [16], but the Ter River detected a high concentration of 97 ng/L [80].
above 1000 ng/L was detected in Wangyang River [62], Ravi River [75] and Kenya [73].
RTM is one of the most concerning antibiotics [28]. The average concentration of RTM
in this study is much lower than that in German [76] and Australian rivers [77], and the
concentration range is equivalent to that in Chenhu Lake [78] and Songhua River [79]. The
detected concentration of CLR in other watersheds is low, basically at the level of 1–10
ng/L, such as the Jialing River in Chongqing [54] and the Chester River in the United States
[16], but the Ter River detected a high concentration of 97 ng/L [80].
Figure 5 and Table S5 list the occurrence of eight antibiotics in other different areas in
wet season.Figure
Similar 5 to
andtheTable S5 list the occurrence
above-mentioned of eight
circumstance, thisantibiotics in other
study selected the datadifferent
meas- areas
ured inin wet
wet season.
season forSimilar to the above-mentioned
comparison (Supplementary Table circumstance,
S5). It is this study
worth notingselected the data
that the
classes of antibiotic measured in this study area are SAs and MCs, with low concentrations, that
measured in wet season for comparison (Supplementary Table S5). It is worth noting
similarthe
to classes of antibiotic
aquaculture measured
farms [18], while the inmain
this study area in
antibiotics are SAssediment
other and MCs, with low concen-
environments
trations, similar to aquaculture farms [18], while the main antibiotics
are QNs and TCs [81]. SMX was the most frequently detected antibiotic in SAs. Except in other sediment
for
environments are QNs and TCs [81]. SMX was the most frequently
Michigan Lake [40], SMX was detected in other areas, and reached the highest concentration detected antibiotic in
SAs.ng/g
of 118.76 Except for Michigan
in Honghu Lake
Lake [82] and[40], SMXng/g
115.35 wasindetected
Dongting in Lake
other[82].
areas, andbe
It can reached
seen the
highest concentration of 118.76 ng/g in Honghu Lake [82] and 115.35
that the content of SMX in lake sediments in China is relatively high [24], while the SMX ng/g in Dongting
Lake [82]. It can be seen that the content of SMX in lake sediments
pollution in river sediments was relatively light, such as at Fenhe River [83] and Liaohe in China is relatively
high [24], while the SMX pollution in river sediments was relatively light,
River [84]. SMZ was detected in the topsoil of Beijing and Shanghai [25], and the concentra- such as at Fenhe
River [83] and Liaohe River [84]. SMZ was detected in the topsoil of
tion was close to the results of this study with the same order of magnitude. A high concen- Beijing and Shang-
hai [25], and the concentration was close
tration of 59 ng/g was measured in the Haihe River [85]. to the results of this study with the same order of
magnitude. A high concentration of 59 ng/g was measured in the Haihe River [85].
Figure 5. Comparison of target antibiotic concentrations in sediment in different regions.

Figure 5. Comparison of target antibiotic concentrations in sediment in different regions.
The detection frequency of MC antibiotics was low, but some studies have detected
highdetection
The concentrations and have
frequency of MCshown that these
antibiotics wasarelow,thebut
main pollutants
some studies in sediments
have [21,23].
detected
high For example, 5620
concentrations andng/g
have and 2582that
shown ng/g of RTM
these are thewere detected
main in Haihe
pollutants River [85] and
in sediments
Wangyang
[21,23]. River5620
For example, [62], ng/g
respectively.
and 2582 Inng/g
contrast, less than
of RTM were10 ng/g ofin
detected RTMHaihewasRiver
detected
[85]in this
study, similar
and Wangyang to [62],
River the Huangpu River
respectively. In [11] and La
contrast, Poudre
less than 10River
ng/g[70]. It is was
of RTM worth mentioning
detected
that the Suzhou Creek flows into the Huangpu River, the antibiotic concentration of Suzhou
Creek dominated the antibiotic pollution of Huangpu River to a certain extent [29]. The
concentration levels of other MC antibiotics (CLR and AZM) detected in this study were
basically consistent with those in Jianghan Plain [86] and Chenhu Lake [78] at a low level.
As Figure 6 shows, compared with the concentration of antibiotics reported in Shang-
hai, the concentration of antibiotics detected in Suzhou Creek is low, and detected antibiotics
have been discussed in previous studies on Shanghai as well. Notably, the concentrations
of those antibiotics in water from this study were significantly lower than those reported
from previous studies [87,88]. Further, the concentration of these antibiotics showed a
decreasing trend, the reason for which may be that the government has carried out the
regulation works in relevant river sections in 2020. Compared with other densely populated
watersheds, Suzhou Creek shows a low concentration of antibiotic pollution as well [89,90].
3.2. Correlation Analysis and Pseudo Distribution Coefficient

3.2.1. Pearson Correlation Analysis
The Pearson correlation coefficient method was used to analyze the occurrence rela-
tionship of antibiotics in both sediment and surface water in Suzhou Creek. As shown
in Figure 7, it can be seen that there is a very significant positive correlation between
multiple pairs of antibiotics in the water body (p < 0.01), such as SPD and SMX, CLR and
RTM, EM and CLR. There is also a very significant positive correlation between many
pairs of antibiotics in sediments, such as EM and RTM, CLR and EM, SPD and EM. This
As Figure 6 shows, compared with the concentration of antibiotics reported in Shang-
hai, the concentration of antibiotics detected in Suzhou Creek is low, and detected antibi-
otics have been discussed in previous studies on Shanghai as well. Notably, the concen-
trations of those antibiotics in water from this study were significantly lower than those
Sustainability 2022, 14, 8757 reported from previous studies [87,88]. Further, the concentration of these antibiotics12 of 19
showed a decreasing trend, the reason for which may be that the government has carried
out the regulation works in relevant river sections in 2020. Compared with other densely
populated watersheds, Suzhou Creek shows a low concentration of antibiotic pollution as
suggests that these antibiotics may have the same source and have the same occurrence
well [89,90].
trajectory [11].
Figure 6. Comparison of antibiotic concentrations in surface water between this study and previous
Figure 6. Comparison of antibiotic concentrations in surface water between this study and previous
results from Shanghai.
results from Shanghai.
AZM（S）
AZM(S) 3.2. Correlation Analysis and Pseudo Distribution
CLR（S） Coefficient
1.000
CLR(S) RTM（S）
RTM(S)
3.2.1. Pearson Correlation Analysis EM（S）
1.000 0.6000
SPD（S）
EM(S) The Pearson correlation0.6000coefficient method was used to analyze the occurrence rela-
AZM（W）
CLR（W） 0.2000
SPD(S)
tionship of antibiotics in both sediment and surface water in Suzhou Creek. As shown in
RTM（W）
0.2000
SMZ(S)
Figure 7, it can be seen that there is a very significant positive correlation between multiple
EM（W） -0.2000
SMX(S) −0.2000 SMM（W）
CLR(W)
pairs of antibiotics in the water body (p < 0.01), such as SPD and SMX, CLR and RTM, EM
SPD（W） -0.6000
−0.6000
RTM(W) and CLR. There is also a very significant positive correlation between many pairs of anti-
TMP（W）
SCP（W）
-1.000
−1.000
SPD(W) biotics in sediments, such as EM and RTM, SMR（W） CLR and EM, SPD and EM. This suggests that
SDZ（W）
SMX(W)
these antibiotics may have the same source SMX（W） and have the same occurrence trajectory [11].
OFL(W)
））））））））））） S） S） S） S） S）
W W W W W W W W W W W
（（（（ P （（（（（ R （（ D （ M（ M（ R （ M（
X DZ R CP D
M SP MM EM TM CL ZM SP E RT CL AZ
SM S SM S T S R A
(a) (b)
Figure
Figure 7.7. Pearson
Pearsoncorrelation
correlationanalysis
analysisofofantibiotic
antibioticconcentrations
concentrationsin in
surface water
surface and
water sediment
and sedimentin
Suzhou Creek: (a) correlation analysis of antibiotics in wet season; (b) correlation analysis
in Suzhou Creek: (a) correlation analysis of antibiotics in wet season; (b) correlation analysis ofof antibi-
otics in dry season.
antibiotics in dry season.
3.2.2.
3.2.2. Pseudo
Pseudo Distribution
Distribution Coefficient
Coefficient
The
The pseudo distribution
distributioncoefficient
coefficient[70],
[70],that
thatis,is,the
theratio
ratioofof
thethe measured
measured concentra-
concentration
tion in sediments
in sediments to corresponding
to the the corresponding concentration
concentration in surface
in surface water,
water, is used
is used to describe
to describe the
the dynamic
dynamic changes
changes of antibiotics
of antibiotics in sediment
in sediment andand
waterwater [91].
[91]. Considering
Considering thethe difference
difference of
detection
of detectionfrequency
frequency between
betweenwater and and
water sediment,
sediment,antibiotics with with
antibiotics a detection frequency
a detection fre-
greater greater
quency than 50% thanin both
50% insurface water and
both surface water sediment
and sedimentwere selected to calculate
were selected Kd value.
to calculate Kd
Four kinds
value. Four of antibiotics
kinds were detected
of antibiotics in wetinseason,
were detected wet season,and five
andkinds of antibiotics
five kinds were
of antibiotics
detected
were in dryinseason.
detected dry season.
The K value
The Kdd value of ofSMX
SMXin inSupplementary
SupplementaryTable Table S6 S6 and
and AZMAZM in in Supplementary
Supplementary Table Table
S7 are relatively high, indicating that mentioned antibiotics are easier
S7 are relatively high, indicating that mentioned antibiotics are easier to adsorb on the to adsorb on the
sediment. In
sediment. In other
other words,
words, compared
compared withwith thethe aquatic
aquatic environment,
environment, SMX SMX and and AZM
AZM are are
easier to
easier toaffect
affectthe
theecological
ecologicalbalance
balanceofofthe the sediment
sediment [92].
[92]. TheTheKd K d values
values of the
of the rest rest of
of the
the antibiotics
antibiotics are low,
are low, whichwhich
means means that are
that they theymore
are morelikelylikely to in
to exist exist in surface
surface water.water.
Gen-
Generally
erally speaking,
speaking, the the difference
difference ofd Kcan
of K d can
bebe attributed
attributed totothe
thephysicochemical
physicochemicalproperties
properties
of antibiotics (e.g., solubility, molecular structure and hydrophobicity)
of antibiotics (e.g., solubility, molecular structure and hydrophobicity) and the properties and the properties
of surface
of surface water
water and
and sediment
sediment [32,93–95].
[32,93–95].
3.3. Ecological Risk Assessment

The RQ values of most antibiotics in a water body are between 0.01 and 1 [66,96,97],
indicating a certain risk to the water environment. Different types of aquatic organisms
may be exposed to numerous types of antibiotics in the environment. The acute toxicity
of antibiotics was mainly for Daphnia and green algae [42], while Daphnia was more sen-
sitive to chronic toxicity of antibiotics compared to both algae and fish [98–100]. Therefore,
3.3. Ecological Risk Assessment

The RQ values of most antibiotics in a water body are between 0.01 and 1 [66,96,97],
indicating a certain risk to the water environment. Different types of aquatic organisms
may be exposed to numerous types of antibiotics in the environment. The acute toxicity of
antibiotics was mainly for Daphnia and green algae [42], while Daphnia was more sensitive
to chronic toxicity of antibiotics compared to both algae and fish [98–100]. Therefore, timely
monitoring and accurate risk characterization of these pollutants should be carried out.
Considering the worst case, the PNEC value of the most sensitive species in the biological
grade is selected to calculate RQ in this study. Specific acute and chronic toxicity data are
shown in Supplementary Table S8. The results of this study are consistent with previous
research, and shared similar trends as in previous research.
In general, the risk of all antibiotics detected in Suzhou Creek to fish, daphnia and algae
was either low or insignificant. Compared with other regions with the same characteristics
of high population density and wide antibiotic consumption, the ecological risk posed
by antibiotics in Suzhou Creek was obviously at a low level [34,44,85]. Compared with
previous studies in the same region, the results were basically consistent [29]. As shown
in Figure 8, the acute toxicity of antibiotics in wet season was mainly against algae, while
the chronic toxicity was mainly against daphnia. Due to being in different layers of
the foodthe
chain,
foodalgae
chain,are veryare
algae sensitive to antibiotics
very sensitive [44], daphnia
to antibiotics has low
[44], daphnia hastolerance to to an-
low tolerance
antibiotics [98], and
tibiotics [98],fish
andare least
fish aresensitive to antibiotic
least sensitive toxicity
to antibiotic [42]. Specifically,
toxicity in terms
[42]. Specifically, in terms of
of chronic toxicity,
chronic daphnia
toxicity, are more
daphnia sensitive
are more to SAs.
sensitive In terms
to SAs. of acute
In terms toxicity,
of acute algae
toxicity, areare more
algae
more sensitive to MCs. For example, CLR was at
sensitive to MCs. For example, CLR was at median riskmedian risk and had a detection rate
detection rate of 100%,
of 100%,while
whileSMX SMXand andTMP,
TMP,belonging
belonging to to
SA,SA,
had had a relatively
a relatively lowlow detection
detection rate rate and risk.
and low
low risk.
P17
P16
P15
P14
P13
High risk
P12
P11
Median risk
P10
P9
Low risk
P8
P7
Insignificant risk
P6
P5
P4
P3
P2
P1
SMM
RTM
CLR
SMM
RTM
CLR
SMM
RTM
CLR
SMM
RTM
CLR
SMM
RTM
CLR
SMM
RTM
CLR
OFL
TMP
SMX
OFL
TMP
OFL
TMP
SMX
OFL
TMP
OFL
TMP
SPD
SMX
SPD
SPD
SMX
OFL
TMP
SPD
SMX
SPD
SMX
SPD
Fish Daphnia Alage Fish Daphnia Alage

Acute toxicity Chronic toxicity
Figure 8. Heat map of RQ values of antibiotics in surface water in wet season. P1 (Wetland Park),
P2 (Fishing center), P3 (Golf Club), P4 (Wusong River Bridge), P5 (Shuangyang port), P6 (Huajiang
Figure 8. Heat map of RQ values of antibiotics in surface water in wet season. P1 (Wetland Park),
bridge), P7 (Tongpu road), P8 (Qilianshan bridge), P9 (Sightseeing dock), P10 (Ludinglu bridge),
P11 (Gubeilu bridge),
bridge), P12 (Kaixuanlu
P7 (Tongpu road), bridge), P13 (ECUPL),
P8 (Qilianshan P14P9(Wuninglu
bridge), bridge),
(Sightseeing P15P10
dock), (Zhenpinglu
(Ludinglu bridge),
bridge), P16
P11(Changhualu bridge),
(Gubeilu bridge), P12P17 (Changshoulu
(Kaixuanlu bridge).
bridge), P13 (ECUPL), P14 (Wuninglu bridge), P15 (Zhen-
pinglu bridge), P16 (Changhualu bridge), P17 (Changshoulu bridge).
More kinds and higher concentrations of antibiotics were detected in the dry season,
which also led to akinds
More moreandserious ecological
higher risk level
concentrations than in thewere
of antibiotics wet detected
season (Figure 9). season,
in the dry
Among these,
whichmacrolide
also led toantibiotics presented
a more serious a high level
ecological of ecological
risk level risk.wet
than in the Forseason
example,
(Figure 9).
CLR, which was different from the wet season, presented a median risk to algae,
Among these, macrolide antibiotics presented a high level of ecological risk. Forwhile EMexample,
presented a high
CLR, risk.was
which It was also the
different fromonly
theantibiotic with
wet season, high riska in
presented this study.
median These
risk to algae, while
kinds of antibiotics are commonly used in clinical and family medicine, so the results of
EM presented a high risk. It was also the only antibiotic with high risk in this study. These
the risk quotient demonstrates that the antibiotic pollution in the study area is composed
kinds of antibiotics are commonly used in clinical and family medicine, so the results of
the risk quotient demonstrates that the antibiotic pollution in the study area is composed
mainly of human antibiotics and that the harm of human antibiotics varies according to
the different types of aquatic organisms.

mainly of human antibiotics and that the harm of human antibiotics varies according to the
different types of aquatic organisms.
P21
P20
P19
P18
P17
P16
P15
P14
high risk
P13
P12 median risk
P11
P10
low risk
P9
P8
P7 insignificant risk
P6
P5
P4
P3
P2
P1
SMX
SDZ
SPD
AZM
SMX
SDZ
SPD
AZM
SMX
SDZ
SPD
AZM
EM
RTM
SMR
SMM
EM
RTM
CLR
SMR
SMM
EM
RTM
CLR
SCP
TMP
SCP
TMP
SMR
SCP
TMP
SMM
CLR
SMX
SDZ
SPD
AZM
SMX
SDZ
SPD
AZM
RTM
SMX
SDZ
SPD
AZM
SMR
SMM
EM
RTM
CLR
SCP
TMP
SMR
CLR
SCP
TMP
SMM
EM
SMR
SMM
EM
RTM
CLR
SCP
TMP
Fish Daphnia Algae Fish Daphnia Algae
Acute toxicity chronic toxicity
Figure 9. Heat map of RQ values of antibiotics in surface water in dry season. P1 (Wetland Park),
Figure 9. Heat map of RQ values of antibiotics in surface water in dry season. P1 (Wetland Park),
bridge), P7 (Tongpu
bridge), road), P8 (Qilianshan
P7 (Tongpu bridge), P9
road), P8 (Qilianshan (Sightseeing
bridge), dock), P10
P9 (Sightseeing (Ludinglu
dock), bridge),
P10 (Ludinglu bridge),
P11 (Gubeilu bridge), P12 (Kaixuanlu
P11 (Gubeilu bridge), P12bridge), P13 (ECUPL),
(Kaixuanlu P14
bridge), P13 (Wuninglu
(ECUPL), P14 bridge),
(Wuninglu P15bridge),
(Zhenpinglu
P15 (Zhen-
pinglu bridge),
bridge), P16 (Changhualu P16 (Changhualu
bridge), bridge),bridge),
P17 (Changshoulu P17 (Changshoulu bridge),
P18 (Guangfu P18
road), (Guangfu
P19 road), P19
(North-south
(North-south viaduct), P20 (Fujianlu bridge), P21 (Garden Bridge).
viaduct), P20 (Fujianlu bridge), P21 (Garden Bridge).
3.4. Identification
3.4. Identification of the
of the Priority Priority Antibiotics
Antibiotics
Sediment
Sediment is both is bothand
the source thesink
source and sink of
of antibiotic antibiotic Some
pollutants. pollutants. Some antibiotics
antibiotics adsorbed ad-
sorbed on the sediment are not easily able to migrate further, while other antibiotics will
on the sediment are not easily able to migrate further, while other antibiotics will be released
be released into surface water and become part of suspended particulate matter for sec-
into surface water and become part of suspended particulate matter for secondary pollution
ondary pollution and diffusion [78]. The sediment plays the role of adsorbing antibiotics
and diffusionbetween
[78]. The sediment
surface water andplays the role ofWith
groundwater. adsorbing antibiotics
the increase of waterbetween surface will
depth, antibiotics
water and groundwater. With the increase of water depth, antibiotics
be captured by sediments, with some antibiotics even penetrating into groundwater, caus-will be captured
by sediments, ingwith
moresomeserious antibiotics evenInpenetrating
pollution [78]. into groundwater,
addition, antibiotic causing
residues in sediments canmore
not only
serious pollution
reflect[78]. In addition,
their migration antibiotic
regularity, residues
but also reflectinthesediments canuse
past antibiotic notinonly reflect
the region [101].
their migration regularity,
Based on previousbut results
also reflect the past
[29,35,44], a new antibiotic
screening use inwas
rule the added
regionunder
[101].the Based
require-
ments of[29,35,44],
on previous results easy operation
a new and accuracy,rule
screening whichwaswas basedunder
added on thetheoccurrence
requirementsof antibiotics
of
easy operation and accuracy, which was based on the occurrence of antibiotics in sediment.anti-
in sediment. The rule takes the detection rate as the screening basis and includes the
The rule takesbiotics that meet the
the detection raterestrictions into the basis
as the screening screening
andprocess.
includes SPDtheand RTM were
antibiotics finally
that
meet the restrictions into the screening process. SPD and RTM were finally selected as in
selected as the priority antibiotics for antibiotic pollution monitoring in Suzhou Creek
wet season. Specific screening conditions and screening process are shown in Supplemen-
the priority antibiotics for antibiotic pollution monitoring in Suzhou Creek in wet season.
tary Table S9. Finally, SPD, EM and CLR were selected as the priority antibiotics for anti-
Specific screening conditions and screening process are shown in Supplementary Table S9.
biotic pollution monitoring in Suzhou Creek in dry season. Specific screening conditions
Finally, SPD,and
EMscreening
and CLRprocesswere selected as the priority antibiotics for antibiotic pollution
are shown in Supplementary Table S10.
monitoring in Suzhou Creek in dry season.
In Europe, spiramycin (SRM) and Specific screening
amoxicillin (AMOX)conditions and in
are included screening
the list of 12
process are shown in Supplementary Table S10.
high ecological risk drugs, and there are six antibiotics among 17 medium ecological risk
In Europe,
drugsspiramycin
[35]. According(SRM) andecological
to the amoxicillin (AMOX) are
risk assessment, included in theroxithromy-
Erythromycin(EM), list of
12 high ecological risk drugs,
cin (RTM) and there are six
and sulfamethoxazole (SMX)antibiotics
have been among 17 medium
identified as threeecological risk
priority antibiotics
drugs [35]. According
in China’s to the ecological
surface risk assessment,
water [5]. Similar to the results Erythromycin(EM),
of this study, RTM poses roxithromycin
median risk to
aquatic organisms in(SMX)
(RTM) and sulfamethoxazole Haihe have
river [85],
been and RTM is identified
identified as threeaspriority
a pollutant of high concern;
antibiotics in
SPDwater
China’s surface has been [5].reported
Similaras tothe
themain
resultsantibiotic
of thisthat brings
study, RTM ecological risk to Poyang
poses median risk toLake
[42]. Itin
aquatic organisms can be seen
Haihe that[85],
river the selected
and RTM priority antibiotics
is identified as are representative.
a pollutant of high It concern;
is worth not-
ing that EM and CLR have been added to the observation
SPD has been reported as the main antibiotic that brings ecological risk to Poyang Lake list of the European Community
[42].
in the field of water policy [102].
It can be seen that the selected priority antibiotics are representative. It is worth noting that
EM and CLR have been added to the observation list of the European Community in the
field of water policy [102].
4. Conclusions
Antibiotics are ubiquitous in surface water all over the world, often detected in the
range of ng/L and ng/g, and pose a potential threat to the ecological environment. This
paper studied the antibiotic pollution status of Suzhou Creek located in a densely populated
urban environment. Compared with other typical surface water environments around the
world, the pollution level of this area is fairly low, and the main types of antibiotics are
SAs and MCs used mostly in clinics and families. Pearson correlation analysis showed
that there was a very significant correlation between multiple groups of antibiotics, which
means that these antibiotics are likely to share a similar emission trajectory. The results of
environment risk assessment show that only EM belongs to high risk level, and the other
antibiotics generally belong to median risk, low risk and no risk level.
Taking into account the occurrence in the sediment and using the optimized priority
screening methods, CLR and RTM were selected as priority antibiotics in wet season, while
SPD, EM and CLR were selected in dry season. Due to the different structure, concentration
and use of each antibiotic, it is necessary to continuously monitor them and optimize the
priority screening rules in order to adapt to the antibiotic pollution with high sensitivity
and rapid change. Though the selected area of this study is small, it may be a starting
point, which is helpful to understand the environmental pollution caused by antibiotics in
urbanized rivers, to further consider their impact on natural water bodies, and to provide
reference for water quality management and antibiotic pollution control in urban areas.
Supplementary Materials: The following are available online at https://www.mdpi.com/article/10

.3390/su14148757/s1, Table S1. Coordinates of sampling sites in Suzhou Creek. Table S2. Gradient
elution conditions of liquid chromatography. Table S3. Monitoring ion pairs and collision energy of
target compounds. Table S4 Comparison of antibiotic occurrence in surface water at home and abroad.
Table S5. Comparison of target antibiotic concentration range in sediment in different regions. Table
S6. Pseudo partition coefficient of antibiotics in wet season. Table S7. Pseudo partition coefficient of
antibiotics in dry season. Table S8. Summary of acute and toxicity data obtained by ECOSAR and
other studies. Table S9. Criteria for the priority antibiotics in Suzhou Creek in wet season. Table S10.
Criteria for the priority antibiotics in Suzhou Creek in dry season.
Author Contributions: Conceptualization, X.L. (Xuhui Li) and X.W.; methodology, X.L. (Xuhui Li) and
X.W.; software, X.L. (Xuhui Li); validation, X.W.; formal analysis, X.L. (Xuhui Li) and X.W.; investigation,
X.L. (Xuhui Li); resources, X.W.; data curation, X.L. (Xuhui Li) and X.W.; writing—original draft
preparation, X.L. (Xuhui Li); writing—review and editing, X.L. (Xuhui Li), Y.Y., D.Z., X.L. (Xiao Li),
D.L. and X.W.; visualization, X.L. (Xuhui Li); supervision, X.W.; project administration, X.W.; funding
acquisition, X.W. All authors have read and agreed to the published version of the manuscript.
Funding: This research was funded by the National Key Research and Development Program of
China (grant numbers 2016YFC0502705); the National Social Science Major Foundation of China
(grant number 14ZDB140), and Major Program of Social Science Foundation of National Education
Ministry of China (20JZD058).
Informed Consent Statement: Not applicable.
Conflicts of Interest: The authors declare no conflict of interest.
References
1. Gould, I.M.; MacKenzie, F.M.; Struelens, M.J.; Meer, J.M.W.V.D. Towards a European strategy for controlling antibiotic resistance
Nijmegen, Holland August 29–31, 1999. Clin. Microbiol. Infect. 2000, 6, 670–674. [CrossRef] [PubMed]
2. Klein, E.Y.; Van Boeckel, T.P.; Martinez, E.M.; Pant, S.; Gandra, S.; Levin, S.A.; Goossens, H.; Laxminarayan, R. Global increase
and geographic convergence in antibiotic consumption between 2000 and 2015. Proc. Natl. Acad. Sci. USA 2018, 115, E3463–E3470.
[CrossRef] [PubMed]
3. Zhang, Q.-Q. Comprehensive evaluation of antibiotics emission and fate in the river basins of China: Source analysis, multimedia
modeling, and linkage to bacterial resistance. Environ. Sci. Technol. 2015, 49, 11. [CrossRef] [PubMed]
4. Kümmerer, K. Antibiotics in the aquatic environment—A review–Part I. Chemosphere 2008, 75, 417–434. [CrossRef] [PubMed]
5. Bu, Q.; Wang, B.; Huang, J.; Deng, S.; Yu, G. Pharmaceuticals and personal care products in the aquatic environment in China: A
review. J. Hazard. Mater. 2013, 262, 189–211. [CrossRef]
6. Phillips, P.J.; Smith, S.G.; Kolpin, D.W.; Zaugg, S.D.; Buxton, H.T.; Furlong, E.T.; Esposito, K.; Stinson, B. Pharmaceutical
Formulation Facilities as Sources of Opioids and Other Pharmaceuticals to Wastewater Treatment Plant Effluents. Environ. Sci.
Technol. 2010, 44, 4910–4916. [CrossRef]
7. Ying, L.; Jingfeng, G.; Yuwei, W.; Wanjun, D.; Jie, L.; Yi, Z.; Haoran, Z.; Mingyan, Z. The removal of antibiotic resistant bacteria
and genes and inhibition of the horizontal gene transfer by contrastive research on sulfidated nanoscale zerovalent iron activating
peroxymonosulfate or peroxydisulfate. J. Hazard. Mater. 2022, 423, 126866.
8. Zhang, R.J.; Yu, K.F.; Li, A.; Wang, Y.H.; Pan, C.G.; Huang, X.Y. Antibiotics in coral reef fishes from the South China Sea:
Occurrence, distribution, bioaccumulation, and dietary exposure risk to human. Sci. Total Environ. 2020, 704, 135288. [CrossRef]
9. Azanu, D.; Styrishave, B.; Darko, G.; Weisser, J.J.; Abaidoo, R.C. Occurrence and risk assessment of antibiotics in water and lettuce
in Ghana. Sci. Total Environ. 2018, 622, 293–305. [CrossRef]
10. Wang, H.X.; Wang, N.; Wang, B.; Zhao, Q.; Fang, H.; Fu, C.W.; Tang, C.X.; Jiang, F.; Zhou, Y.; Chen, Y.; et al. Antibiotics in
Drinking Water in Shanghai and Their Contribution to Antibiotic Exposure of School Children. Environ. Sci. Technol. 2016, 50,
2692–2699. [CrossRef]
11. Singh, R.; Singh, A.P.; Kumar, S.; Giri, B.S.; Kim, K.-H. Antibiotic resistance in major rivers in the world: A systematic review on
occurrence, emergence, and management strategies. J. Clean. Prod. 2019, 234, 1484–1505. [CrossRef]
12. Kairigo, P.; Ngumba, E.; Sundberg, L.-R.; Gachanja, A.; Tuhkanen, T. Occurrence of antibiotics and risk of antibiotic resistance
evolution in selected Kenyan wastewaters, surface waters and sediments. Sci. Total Environ. 2020, 720, 137580. [CrossRef]
[PubMed]
13. Boger, B.; Surek, M.; Vilhena, R.D.; Fachi, M.M.; Junkert, A.M.; Santos, J.; Domingos, E.L.; Cobre, A.D.; Momade, D.R.; Pontarolo,
R. Occurrence of antibiotics and antibiotic resistant bacteria in subtropical urban rivers in Brazil. J. Hazard. Mater. 2021, 402,
123448. [CrossRef] [PubMed]
14. Dinh, Q.T.; Moreau-Guigon, E.; Labadie, P.; Alliot, F.; Teil, M.J.; Blanchard, M.; Chevreuil, M. Occurrence of antibiotics in rural
catchments. Chemosphere 2017, 168, 483–490. [CrossRef] [PubMed]
15. Sabri, N.A.; Schmitt, H.; Van der Zaan, B.; Gerritsen, H.W.; Zuidema, T.; Rijnaarts, H.H.M.; Langenhoff, A.A.M. Prevalence of
antibiotics and antibiotic resistance genes in a wastewater effluent-receiving river in the Netherlands. J. Environ. Chem. Eng. 2020,
8, 102245. [CrossRef]
16. He, K.; Hain, E.; Timm, A.; Tarnowski, M.; Blaney, L. Occurrence of antibiotics, estrogenic hormones, and UV-filters in water,
sediment, and oyster tissue from the Chesapeake Bay. Sci. Total Environ. 2019, 650, 3101–3109. [CrossRef]
17. Chen, Y.; Xie, Q.M.; Wan, J.Q.; Yang, S.; Wang, Y.; Fan, H.M. Occurrence and risk assessment of antibiotics in multifunctional
reservoirs in Dongguan, China. Environ. Sci. Pollut. Res. 2020, 27, 13565–13574. [CrossRef]
18. Han, Q.F.; Zhao, S.; Zhang, X.R.; Wang, X.L.; Song, C.; Wang, S.G. Distribution, combined pollution and risk assessment of
antibiotics in typical marine aquaculture farms surrounding the Yellow Sea, North China. Environ. Int. 2020, 138, 105551.
[CrossRef]
19. Zhang, R.; Tang, J.; Li, J.; Cheng, Z.; Chaemfa, C.; Liu, D.; Zheng, Q.; Song, M.; Luo, C.; Zhang, G. Occurrence and risks of
antibiotics in the coastal aquatic environment of the Yellow Sea, North China. Sci. Total Environ. 2013, 450–451, 197–204. [CrossRef]
20. Lu, J.; Wu, J.; Zhang, C.; Zhang, Y.; Lin, Y.; Luo, Y. Occurrence, distribution, and ecological-health risks of selected antibiotics in
coastal waters along the coastline of China. Sci. Total Environ. 2018, 644, 1469–1476. [CrossRef]
21. Li, W.; Shi, Y.; Gao, L.; Liu, J.; Cai, Y. Occurrence of antibiotics in water, sediments, aquatic plants, and animals from Baiyangdian
Lake in North China. Chemosphere 2012, 89, 1307–1315. [CrossRef] [PubMed]
22. Wu, M.H.; Que, C.J.; Xu, G.; Sun, Y.F.; Ma, J.; Xu, H.; Sun, R.; Tang, L. Occurrence, fate and interrelation of selected antibiotics in
sewage treatment plants and their receiving surface water. Ecotoxicol. Environ. Saf. 2016, 132, 132–139. [CrossRef] [PubMed]
23. Deng, W.J.; Li, N.; Ying, G.G. Antibiotic distribution, risk assessment, and microbial diversity in river water and sediment in
Hong Kong. Environ. Geochem. Health 2018, 40, 2191–2203. [CrossRef] [PubMed]
24. Xu, J.; Zhang, Y.; Zhou, C.; Guo, C.; Wang, D.; Du, P.; Luo, Y.; Wan, J.; Meng, W. Distribution, sources and composition of
antibiotics in sediment, overlying water and pore water from Taihu Lake, China. Sci. Total Environ. 2014, 497–498, 267–273.
[CrossRef] [PubMed]
25. Gao, L.H.; Shi, Y.L.; Li, W.H.; Liu, J.M.; Cai, Y.Q. Occurrence and distribution of antibiotics in urban soil in Beijing and Shanghai,
China. Environ. Sci. Pollut. Res. 2015, 22, 11360–11371. [CrossRef]
26. Reichert, G.; Hilgert, S.; Fuchs, S.; Azevedo, J.C.R. Emerging contaminants and antibiotic resistance in the different environmental
matrices of Latin America. Environ. Pollut. 2019, 255, 113140. [CrossRef]
27. Zhu, Y.G.; Zhao, Y.; Li, B.; Huang, C.L.; Zhang, S.Y.; Yu, S.; Chen, Y.S.; Zhang, T.; Gillings, M.R.; Su, J.Q. Continental-scale
pollution of estuaries with antibiotic resistance genes. Nat. Microbiol. 2017, 2, 16270. [CrossRef]
28. Li, Z.; Li, M.; Zhang, Z.Y.; Li, P.; Zang, Y.G.; Liu, X. Antibiotics in aquatic environments of China: A review and meta-analysis.
Ecotoxicol. Environ. Saf. 2020, 199, 110668. [CrossRef]
29. Zhu, F.; Wang, S.Q.; Liu, Y.J.; Wu, M.H.; Wang, H.Y.; Xu, G. Antibiotics in the surface water of Shanghai, China: Screening,
distribution, and indicator selecting. Environ. Sci. Pollut. Res. 2021, 28, 9836–9848. [CrossRef]
30. Zhou, L.-J.; Ying, G.-G.; Zhao, J.-L.; Yang, J.-F.; Wang, L.; Yang, B.; Liu, S. Trends in the occurrence of human and veterinary
antibiotics in the sediments of the Yellow River, Hai River and Liao River in northern China. Environ. Pollut. 2011, 159, 1877–1885.
[CrossRef]
31. Wen, X.; Feng, Q.; Lu, J.; Wu, J.; Wu, M.; Guo, X. Risk assessment and source identification of coastal groundwater nitrate in
northern China using dual nitrate isotopes combined with Bayesian mixing model. Hum. Ecol. Risk Assess. Int. J. 2018, 24,
1043–1057. [CrossRef]
32. Chen, C.Q.; Zheng, L.; Zhou, J.L.; Zhao, H. Persistence and risk of antibiotic residues and antibiotic resistance genes in major
mariculture sites in Southeast China. Sci. Total Environ. 2017, 580, 1175–1184. [CrossRef] [PubMed]
33. Boxall, A.B.A.; Sinclair, C.J.; Fenner, K.; Kolpin, D.; Maud, S.J. When synthetic chemicals degrade in the environment. Environ. Sci.
Technol. 2004, 38, 368A–375A. [CrossRef] [PubMed]
34. Li, S.; Shi, W.; Li, H.; Xu, N.; Zhang, R.; Chen, X.; Sun, W.; Wen, D.; He, S.; Pan, J.; et al. Antibiotics in water and sediments of
rivers and coastal area of Zhuhai City, Pearl River estuary, south China. Sci. Total Environ. 2018, 636, 1009–1019. [CrossRef]
[PubMed]
35. Zhou, S.B.; Di Paolo, C.; Wu, X.; Shao, Y.; Seiler, T.B.; Hollert, H. Optimization of screening-level risk assessment and priority
selection of emerging pollutants-The case of pharmaceuticals in European surface waters. Environ. Int. 2019, 128, 1–10. [CrossRef]
36. Muir, D.C.G.; Howard, P.H. Are there other persistent organic pollutants? A challenge for environmental chemists. Environ. Sci.
Technol. 2006, 40, 7157–7166. [CrossRef]
37. Sun, S.N.; Chen, Y.A.; Lin, Y.J.; An, D. Occurrence, spatial distribution, and seasonal variation of emerging trace organic pollutants
in source water for Shanghai, China. Sci. Total Environ. 2018, 639, 1–7. [CrossRef]
38. Chen, K.; Zhou, J.L. Occurrence and behavior of antibiotics in water and sediments from the Huangpu River, Shanghai, China.
Chemosphere 2014, 95, 604–612. [CrossRef]
39. Qinqin, Z.; Ai, J.; Yi, W.; Hong, L.; Kunping, W.; Hui, P.; Zhaomin, D.; Jianying, H. Occurrences of three classes of antibiotics in a
natural river basin: Association with antibiotic-resistant Escherichia coli. Environ. Sci. Technol. 2014, 48, 14317–14325.
40. Blair, B.D.; Crago, J.P.; Hedman, C.J.; Klaper, R.D. Pharmaceuticals and personal care products found in the Great Lakes above
concentrations of environmental concern. Chemosphere 2013, 93, 2116–2123. [CrossRef]
41. Wollenberger, L.; Halling-Sorensen, B.; Kusk, K.O. Acute and chronic toxicity of veterinary antibiotics to Daphnia magna.
Chemosphere 2000, 40, 723–730. [CrossRef]
42. Ding, H.J.; Wu, Y.X.; Zhang, W.H.; Zhong, J.Y.; Lou, Q.; Yang, P.; Fang, Y.Y. Occurrence, distribution, and risk assessment of
antibiotics in the surface water of Poyang Lake, the largest freshwater lake in China. Chemosphere 2017, 184, 137–147. [CrossRef]
[PubMed]
43. Hernandoa, M.D.; Mezcuaa, M.; Fernández-Albaa, A.R.; Barceló, D. Environmental risk assessment of pharmaceutical residues in
wastewater effluents, surface waters and sediments. Talanta 2006, 69, 334–342. [CrossRef] [PubMed]
44. Li, F.F.; Chen, Y.J.; Bao, Y.Y.; Zheng, Y.H.; Huang, B.; Mu, Q.L.; Feng, C.P.; Wen, D.H. Identification of the priority antibiotics based
on their detection frequency, concentration, and ecological risk in urbanized coastal water. Sci. Total Environ. 2020, 747, 141275.
[CrossRef] [PubMed]
45. Qin, L.-T.; Pang, X.-R.; Zeng, H.-H.; Liang, Y.-P.; Mo, L.-Y.; Wang, D.-Q.; Dai, J.-F. Ecological and human health risk of sulfonamides
in surface water and groundwater of Huixian karst wetland in Guilin, China. Sci. Total Environ. 2020, 708, 134552. [CrossRef]
46. Ana, P.R.; Beatriz, A.; Macarena, F.; Luis, T.J. Analysis of macrolide antibiotics in water by magnetic solid-phase extraction and
liquid chromatography-tandem mass spectrometry. J. Pharm. Biomed. Anal. 2017, 146, 79–85.
47. Jiao, S.; Zheng, S.; Yin, D.; Wang, L.; Chen, L. Aqueous photolysis of tetracycline and toxicity of photolytic products to luminescent
bacteria. Chemosphere 2008, 73, 377–382. [CrossRef]
48. Dai, Y.J.; Liu, M.; Li, J.J.; Yang, S.S.; Sun, Y.; Sun, Q.Y.; Wang, W.S.; Lu, L.; Zhang, K.X.; Xu, J.Y.; et al. A review on pollution
situation and treatment methods of tetracycline in groundwater. Sep. Sci. Technol. 2020, 55, 1005–1021. [CrossRef]
49. Osinska, A.; Korzeniewska, E.; Harnisz, M.; Felis, E.; Bajkacz, S.; Jachimowicz, P.; Niestepski, S.; Konopka, I. Small-scale
wastewater treatment plants as a source of the dissemination of antibiotic resistance genes in the aquatic environment. J. Hazard.
Mater. 2020, 381, 121221. [CrossRef]
50. Kumar, M.; Jaiswal, S.; Sodhi, K.K.; Shree, P.; Singh, D.K.; Agrawal, P.K.; Shukla, P. Antibiotics bioremediation: Perspectives on its
ecotoxicity and resistance. Environ. Int. 2019, 124, 448–461. [CrossRef]
51. Liang, X.M.; Guan, F.L.; Chen, B.W.; Luo, P.Y.; Guo, C.F.; Wu, G.Q.; Ye, Y.; Zhou, Q.B.; Fang, H.S. Spatial and seasonal variations
of antibiotic resistance genes and antibiotics in the surface waters of Poyang Lake in China. Ecotoxicol. Environ. Saf. 2020, 196,
110543. [CrossRef] [PubMed]
52. Liu, S.; Su, H.C.; Pan, Y.F.; Xu, X.R. Spatial and seasonal variations of antibiotics and antibiotic resistance genes and ecological
risks in the coral reef regions adjacent to two typical islands in South China Sea. Mar. Pollut. Bull. 2020, 158, 111424. [CrossRef]
[PubMed]
53. Stoob, K.; Singer, H.P.; Mueller, S.R.; Schwarzenbach, R.P.; Stamm, C.H. Dissipation and transport of veterinary sulfonamide
antibiotics after manure application to grassland in a small catchment. Environ. Sci. Technol. 2007, 41, 7349–7355. [CrossRef]
[PubMed]
54. Wang, G.; Zhou, S.; Han, X.; Zhang, L.; Ding, S.; Li, Y.; Zhang, D.; Zarin, K. Occurrence, distribution, and source track of
antibiotics and antibiotic resistance genes in the main rivers of Chongqing city, southwest China. J. Hazard. Mater. 2020, 389,
122110. [CrossRef]
55. Li, B.; Zhang, T. Removal mechanisms and kinetics of trace tetracycline by two types of activated sludge treating freshwater
sewage and saline sewage. Environ. Sci. Pollut. Res. 2013, 20, 3024–3033. [CrossRef] [PubMed]
56. Chen, Y.; Hu, C.; Qu, J.; Yang, M. Photodegradation of tetracycline and formation of reactive oxygen species in aqueous
tetracycline solution under simulated sunlight irradiation. J. Photochem. Photobiol. A Chem. 2007, 197, 81–87. [CrossRef]
57. Wammer, K.H.; Korte, A.R.; Lundeen, R.A.; Sundberg, J.E.; McNeill, K.; Arnold, W.A. Direct photochemistry of three fluoro-
quinolone antibacterials: Norfloxacin, ofloxacin, and enrofloxacin. Water Res. 2013, 47, 439–448. [CrossRef]
58. Zhou, L.J.; Li, J.; Zhang, Y.D.; Kong, L.Y.; Jin, M.; Yang, X.D.; Wu, Q.L.L. Trends in the occurrence and risk assessment of antibiotics
in shallow lakes in the lower-middle reaches of the Yangtze River basin, China. Ecotoxicol. Environ. Saf. 2019, 183, 109511.
[CrossRef]
59. Anke, G.; Angela, T.; McArdell, C.S.; Adriano, J.; Walter, G. Occurrence and sorption behavior of sulfonamides, macrolides, and
trimethoprim in activated sludge treatment. Environ. Sci. Technol. 2005, 39, 3981–3989.
60. Kafaei, R.; Papari, F.; Seyedabadi, M.; Sahebi, S.; Tahmasebi, R.; Ahmadi, M.; Sorial, G.A.; Asgari, G.; Ramavandi, B. Occurrence,
distribution, and potential sources of antibiotics pollution in the water-sediment of the northern coastline of the Persian Gulf,
Iran. Sci. Total Environ. 2018, 627, 703–712. [CrossRef]
61. Tran, N.H.; Chen, H.J.; Reinhard, M.; Mao, F.; Gin, K.Y.H. Occurrence and removal of multiple classes of antibiotics and
antimicrobial agents in biological wastewater treatment processes. Water Res. 2016, 104, 461–472. [CrossRef] [PubMed]
62. Jiang, Y.H.; Li, M.X.; Guo, C.S.; An, D.; Xu, J.; Zhang, Y.; Xi, B.D. Distribution and ecological risk of antibiotics in a typical
effluent-receiving river (Wangyang River) in north China. Chemosphere 2014, 112, 267–274. [CrossRef] [PubMed]
63. Carrasquillo, A.J.; Bruland, G.L.; Mackay, A.A.; Vasudevan, D. Sorption of Ciprofloxacin and Oxytetracycline Zwitterions to Soils
and Soil Minerals: Influence of Compound Structure. Environ. Sci. Technol. 2008, 42, 7634–7642. [CrossRef] [PubMed]
64. Li, Z.; Zheng, T.L.; Li, M.; Liu, X. Organic contaminants in the effluent of Chinese wastewater treatment plants. Environ. Sci.
Pollut. Res. 2018, 25, 26852–26860. [CrossRef]
65. Jerker, F.; Hanna, S.; Lindberg, R.H.; Chau, P.; Mats, T.; Joakim, L.D.G. Contamination of surface, ground, and drinking water
from pharmaceutical production. Environ. Toxicol. Chem. 2009, 28, 2522–2527.
66. Deng, W.J.; Li, N.; Zheng, H.L.; Lin, H.Y. Occurrence and risk assessment of antibiotics in river water in Hong Kong. Ecotoxicol.
Environ. Saf. 2016, 125, 121–127. [CrossRef]
67. Murata, A.; Takada, H.; Mutoh, K.; Hosoda, H.; Harada, A.; Nakada, N. Nationwide monitoring of selected antibiotics:
Distribution and sources of sulfonamides, trimethoprim, and macrolides in Japanese rivers. Sci. Total Environ. 2011, 409,
5305–5312. [CrossRef]
68. Jia, A.; Hu, J.Y.; Wu, X.Q.; Peng, H.; Wu, S.M.; Dong, Z.M. Occurrence and Source Apportionment of sulfonamides and Their
Metabolites in Liaodong Bay and the Adjacent Liao River Basin, North China. Environ. Toxicol. Chem. 2011, 30, 1252–1260.
[CrossRef]
69. Feng, J.L.; Liu, Q.; Ru, X.L.; Xi, N.N.; Sun, J.H. Occurrence and distribution of priority pharmaceuticals in the Yellow River and
the Huai River in Henan, China. Environ. Sci. Pollut. Res. 2020, 27, 16816–16826. [CrossRef]
70. Kim, S.C.; Carlson, K. Temporal and spatial trends in the occurrence of human and veterinary antibiotics in aqueous and river
sediment matrices. Environ. Sci. Technol. 2007, 41, 50–57. [CrossRef]
71. Lei, K.; Zhu, Y.; Chen, W.; Pan, H.Y.; Cao, Y.X.; Zhang, X.; Guo, B.B.; Sweetman, A.; Lin, C.Y.; Ouyang, W.; et al. Spatial and
seasonal variations of antibiotics in river waters in the Haihe River Catchment in China and ecotoxicological risk assessment.
Environ. Int. 2019, 130, 104919. [CrossRef] [PubMed]
72. Dinh, Q.T.; Alliot, F.; Moreau-Guigon, E.; Eurin, J.; Chevreuil, M.; Labadie, P. Measurement of trace levels of antibiotics in river
water using on-line enrichment and triple-quadrupole LC-MS/MS. Talanta 2011, 85, 1238–1245. [CrossRef] [PubMed]
73. Ngumba, E.; Gachanja, A.; Tuhkanen, T. Occurrence of selected antibiotics and antiretroviral drugs in Nairobi River Basin, Kenya.
Sci. Total Environ. 2016, 539, 206–213. [CrossRef]
74. Suzuki, S.; Ogo, M.; Koike, T.; Takada, H.; Newman, B. Sulfonamide and tetracycline resistance genes in total- and culturable-
bacterial assemblages in South African aquatic environments. Front. Microbiol. 2015, 6, 796. [CrossRef] [PubMed]
75. Khan, G.A.; Berglund, B.; Khan, K.M.; Lindgren, P.-E.; Fick, J. Occurrence and abundance of antibiotics and resistance genes in
rivers, canal and near drug formulation facilities–a study in Pakistan. PLoS ONE 2017, 8, e62712. [CrossRef] [PubMed]
76. Hirsch, R.; Ternes, T.; Haberer, K.; Kratz, K.L. Occurrence of antibiotics in the aquatic environment. Sci. Total Environ. 1999, 225,
109–118. [CrossRef]
77. Watkinson, A.J.; Murby, E.J.; Kolpin, D.W.; Costanzo, S.D. The occurrence of antibiotics in an urban watershed: From wastewater
to drinking water. Sci. Total Environ. 2009, 407, 2711–2723. [CrossRef]
78. Ma, N.; Tong, L.; Li, Y.; Yang, C.; Tan, Q.; He, J. Distribution of antibiotics in lake water-groundwater-Sediment system in Chenhu
Lake area. Environ. Res. 2022, 204 Pt C, 112343. [CrossRef]
79. Wang, W.H.; Wang, H.; Zhang, W.F.; Liang, H.; Gao, D.W. Occurrence, distribution, and risk assessment of antibiotics in the
Songhua River in China. Environ. Sci. Pollut. Res. 2017, 24, 19282–19292. [CrossRef]
80. Rodriguez-Mozaz, S.; Chamorro, S.; Marti, E.; Huerta, B.; Gros, M.; Sanchez-Melsio, A.; Borrego, C.M.; Barcelo, D.; Balcazar, J.L.
Occurrence of antibiotics and antibiotic resistance genes in hospital and urban wastewaters and their impact on the receiving
river. Water Res. 2015, 69, 234–242. [CrossRef]
81. Liu, X.H.; Lu, S.Y.; Guo, W.; Xi, B.D.; Wang, W.L. Antibiotics in the aquatic environments: A review of lakes, China. Sci. Total
Environ. 2018, 627, 1195–1208. [CrossRef] [PubMed]
82. Yang, Y.Y.; Cao, X.H.; Lin, H.; Wang, J. Antibiotics and Antibiotic Resistance Genes in Sediment of Honghu Lake and East
Dongting Lake, China. Microb. Ecol. 2016, 72, 791–801. [CrossRef] [PubMed]
83. Zhu, Y.; Miao, J.R.; Wen, H.X.; Li, T.H.X.; Zhao, Z.H.; Guo, X.; Li, H.; Zhang, G.X. The occurrence and spatial distribution of
typical antibiotics in soils along the Fenhe River in Shanxi Province. J. Soils Sediments 2020, 20, 889–899. [CrossRef]
84. Xu, Y.; Guo, C.S.; Lv, J.P.; Hou, S.; Luo, Y.; Zhang, Y.; Xu, J. Spatiotemporal profile of tetracycline and sulfonamide and their
resistance on a catchment scale. Environ. Pollut. 2018, 241, 1098–1105. [CrossRef] [PubMed]
85. Chen, H.Y.; Jing, L.J.; Teng, Y.G.; Wang, J.S. Characterization of antibiotics in a large-scale river system of China: Occurrence
pattern, spatiotemporal distribution and environmental risks. Sci. Total Environ. 2018, 618, 409–418. [CrossRef]
86. Tong, L.; Qin, L.T.; Xie, C.; Liu, H.X.; Wang, Y.X.; Guan, C.A.; Huang, S.B. Distribution of antibiotics in alluvial sediment near
animal breeding areas at the Jianghan Plain, Central China. Chemosphere 2017, 186, 100–107. [CrossRef]
87. He, Y.; Tang, Y.Y.; Sun, F.J.; Chen, L.M. Detection and characterization of integrative and conjugative elements (ICEs)-positive
Vibrio cholerae isolates from aquacultured shrimp and the environment in Shanghai, China. Mar. Pollut. Bull. 2015, 101, 526–532.
[CrossRef]
88. Jiang, L.; Hu, X.L.; Yin, D.Q.; Zhang, H.C.; Yu, Z.Y. Occurrence, distribution and seasonal variation of antibiotics in the Huangpu
River, Shanghai, China. Chemosphere 2011, 82, 822–828. [CrossRef]
89. Yan, C.; Yang, Y.; Zhou, J.; Liu, M.; Nie, M.; Shi, H.; Gu, L. Antibiotics in the surface water of the Yangtze Estuary: Occurrence,
distribution and risk assessment. Environ. Pollut. 2013, 175, 22–29. [CrossRef]
90. Liu, X.; Steele, J.C.; Meng, X.Z. Usage, residue, and human health risk of antibiotics in Chinese aquaculture: A review. Environ.
Pollut. 2017, 223, 161–169. [CrossRef]
91. Wenwen, G.; Xinhui, L.; Hui, H.; Liang, W.; Guohua, D. Quantitatively modeling soil-water distribution coefficients of three
antibiotics using soil physicochemical properties. Chemosphere 2012, 89, 825–831.
92. Radke, M.; Lauwigi, C.; Heinkele, G.; Murdter, T.E.; Letzel, M. Fate of the Antibiotic Sulfamethoxazole and Its Two Major Human
Metabolites in a Water Sediment Test. Environ. Sci. Technol. 2009, 43, 3135–3141. [CrossRef] [PubMed]
93. Liang, X.M.; Chen, B.W.; Nie, X.P.; Shi, Z.; Huang, X.P.; Li, X.D. The distribution and partitioning of common antibiotics in water
and sediment of the Pearl River Estuary, South China. Chemosphere 2013, 92, 1410–1416. [CrossRef]
94. Li, S.; Shi, W.; Liu, W.; Li, H.; Zhang, W.; Hu, J.; Ke, Y.; Sun, W.; Ni, J. A duodecennial national synthesis of antibiotics in China’s
major rivers and seas (2005–2016). Sci. Total Environ. 2018, 615, 906–917. [CrossRef]
95. Luo, Y.; Xu, L.; Rysz, M.; Wang, Y.Q.; Zhang, H.; Alvarez, P.J.J. Occurrence and Transport of Tetracycline, Sulfonamide, Quinolone,
and Macrolide Antibiotics in the Haihe River Basin, China. Environ. Sci. Technol. 2011, 45, 1827–1833. [CrossRef] [PubMed]
96. Wu, X.-L.; Xiang, L.; Yan, Q.-Y.; Jiang, Y.-N.; Li, Y.-W.; Huang, X.-P.; Li, H.; Cai, Q.-Y.; Mo, C.-H. Distribution and risk assessment
of quinolone antibiotics in the soils from organic vegetable farms of a subtropical city, Southern China. Sci. Total Environ. 2014,
487, 399–406. [CrossRef] [PubMed]
97. Wang, J.; Wei, H.; Zhou, X.; Li, K.; Wu, W.; Guo, M. Occurrence and risk assessment of antibiotics in the Xi’an section of the Weihe
River, northwestern China. Mar. Pollut. Bull. 2019, 146, 794–800. [CrossRef] [PubMed]
98. Li, S.; Shi, W.Z.; You, M.T.; Zhang, R.J.; Kuang, Y.Z.; Dang, C.Y.; Sun, W.L.; Zhou, Y.H.; Wang, W.J.; Ni, J.R. Antibiotics in water
and sediments of Danjiangkou Reservoir, China: Spatiotemporal distribution and indicator screening. Environ. Pollut. 2019, 246,
435–442. [CrossRef]
99. Wang, Z.; Du, Y.; Yang, C.; Liu, X.; Zhang, J.Q.; Li, E.H.; Zhang, Q.; Wang, X.L. Occurrence and ecological hazard assessment of
selected antibiotics in the surface waters in and around Lake Honghu, China. Sci. Total Environ. 2017, 609, 1423–1432. [CrossRef]
100. Sun, C.S.; Hu, E.; Liu, S.W.; Wen, L.; Yang, F.; Li, M. Spatial distribution and risk assessment of certain antibiotics in 51 urban
wastewater treatment plants in the transition zone between North and South China. J. Hazard. Mater. 2022, 437, 129307. [CrossRef]
101. Kerrigan, J.F.; Sandberg, K.D.; Engstrom, D.R.; LaPara, T.M.; Arnold, W.A. Sedimentary record of antibiotic accumulation in
Minnesota Lakes. Sci. Total Environ. 2018, 621, 970–979. [CrossRef] [PubMed]
102. Desbiolles, F.; Malleret, L.; Tiliacos, C.; Wong-Wah-Chung, P.; Laffont-Schwob, I. Occurrence and ecotoxicological assessment of
pharmaceuticals: Is there a risk for the Mediterranean aquatic environment? Sci. Total Environ. 2018, 639, 1334–1348. [CrossRef]
[PubMed]

Sustainability 14 08757

Uploaded by

Document Information

Copyright

Available Formats

Share this document

Share or Embed Document

Sharing Options

Did you find this document useful?

Is this content inappropriate?

Copyright:

Available Formats

Sustainability 14 08757

Uploaded by

Copyright:

Available Formats

sustainability

Academic Editor: Antonio

Sustainability 2022, 14, 8757. https://doi.org/10.3390/su14148757 https://www.mdpi.com/journal/sustainability

Many studies have focused on the pollution characteristics of antibiotics around

Sustainability 2022, 14, 8757 3 of 19

In the experiment, HPLC-grade acetonitrile was acquired from Thermofisher (Waltham,

2.3. Sample Pretreatment

2.4. Analytical Methods

2.5. Quality Analysis and Control

2.6. Pseudo Distribution Coefficient

2.7. Environmental Risk Assessment

2.8. Priority Antibiotics Screening Method

3. Results and Discussion

3.1.2. Antibiotics in Sediment

Wet Season (ng/g) Wet Season (ng/g)

Figure 5. Comparison of target antibiotic concentrations in sediment in different regions.

3.2. Correlation Analysis and Pseudo Distribution Coefficient

Sustainability 2022, 14, x FOR PEER REVIEW 13 of 20

SMX(S) −0.2000 SMM（W）

3.3. Ecological Risk Assessment

3.3. Ecological Risk Assessment

Fish Daphnia Alage Fish Daphnia Alage

Sustainability 2022, 14, x FOR PEER REVIEW 15 of 20

Supplementary Materials: The following are available online at https://www.mdpi.com/article/10

You might also like