Marine Pollution Bulletin 182 (2022) 113975

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Marine Pollution Bulletin

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

Spatiotemporal patterns and influencing factors of dissolved heavy metals

off the Yangtze River Estuary, East China Sea
Xupeng Hu a, b, c, Xiaoyong Shi a, d, *, Rongguo Su a, Yimin Jin b, Shijun Ren b, Xinxin Li c, e, *
a
College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao 266100, China
b
Zhejiang Marine Ecology and Environment Monitoring Center, Zhoushan 316021, China
c
Department of Ocean Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
d
National Marine Hazard Mitigation Service, Ministry of Natural Resources, Beijing 100194, China
e
Southern Marine Science and Engineering Guangdong Laboratory (Guangzhou), Guangzhou, 511458, Guangdong, China

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

Keywords: Dissolved heavy metal pollution in the ocean is becoming an environmental concern. Their distribution patterns
East China Sea are complex and influenced by multiple factors in the coastal ocean. Therefore, more investigations are needed to
Dissolved heavy metals understand their behavior in the seawater. This study systematically investigated the distribution of Cu, Pb, Cd,
Spatiotemporal patterns
As, Zn and seawater properties in the surface and bottom water off the Yangtze River Estuary, East China Sea in
Sources
spring, summer and autumn, 2019. The results showed significant spatiotemporal distribution that three-zone-
Hydrodynamics
Biological effect pattern of estuary, nearshore, and offshore can be divided. While sources, hydrodynamics, biological uptake
Resuspension and sediment resuspension affected the overall distribution, dissolved oxygen and pH dominantly influenced the
estuary and offshore respectively, with more complex factors in the nearshore. Low ecological risks were assessed
during the study, but global warming, ocean acidification and hypoxia are essential concerns to understand the
biogeochemistry of dissolved heavy metals in the ocean.

1. Introduction
Dissolved heavy metal pollution has become a global concern due to
their persistence, high toxicity and bioaccumulation (Gao et al., 2014;
Hu et al., 2015; Lao et al., 2019; Liu et al., 2021; Malik et al., 2010; Pan
and Wang, 2012; Park et al., 2020; Sun et al., 2020). The coastal ocean
are especially sensitive to natural changes and anthropogenic pollution
(Zhang et al., 2017b). Weathering and rock erosion were important
natural causes of heavy metal entry to the environment (Haynes and
Johnson, 2000). River and wastewater discharge are also important
sources for the heavy metal contamination (Dai et al., 2009). Anthro­
pogenic activities, particularly electroplating, mining and mineral pro­
cessing, and atmospheric deposition of exhaust gas influence the heavy
metals cycles greatly (Dou et al., 2013; Jiann and Wen, 2009; Wang
et al., 2013; Zhang et al., 2015).
Once entering the ocean, the partition between different phases and
the behaviors of dissolved heavy metals were usually affected by the
seawater properties such as salinity (S), dissolved oxygen (DO), pH,
nutrients, chemical oxygen demand (COD), and suspended particulate
materials (SPM) (Islam et al., 2015; Mohiuddin et al., 2012; Wang et al.,
2012b; Zhang et al., 2020). For example, temperature, DO and pH would
affect the biosorption of dissolved metals directly (Kubilay et al., 2007;
Zhang et al., 2020). Lower DO and pH induced hypoxia and acidification
might enhance the release of dissolved heavy metals (Atkinson et al.,
2007; Banks et al., 2012). Additionally, heavy metals would be released
from sediment due to resuspension and cause a secondary pollution (Du
Laing et al., 2008; Hu et al., 2016; Kang et al., 2017; Liu et al., 2019a;
Zhang et al., 2018; Zhuang and Zhou, 2021).
The East China Sea off the Yangtze River Estuary (YRE) is featured by
a large river-dominated delta (He et al., 2019). Many adjoining semi-
enclosed bays such as Hangzhou Bay (HZB), Xiangshan Harbor (XSH),
Sanmen Bay (SMB) and Yueqing Bay (YQB) accept large quantities of
river discharge and become point sources of pollution (Fig. 1). Along
with the rapid increase of population, industrial and agriculture devel­
opment, the YRE have been facing emerging heavy metal pollution and
ecological and environmental risks (An et al., 2010; Bianchi and Allison,
2009; Pang et al., 2015; Wang et al., 2015; Yin et al., 2015; Zhuang and
Zhou, 2021). Studies have been focusing on the source identification and

* Correspondence to: X. Li, Department of Ocean Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China and X. Shi,
College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao 266100, China.
E-mail addresses: shixy@ouc.edu.cn (X. Shi), lixinxin@sustech.edu.cn (X. Li).

https://doi.org/10.1016/j.marpolbul.2022.113975
Received 9 June 2022; Received in revised form 19 July 2022; Accepted 21 July 2022
Available online 5 August 2022
0025-326X/© 2022 Elsevier Ltd. All rights reserved.
X. Hu et al.
risk assessment of heavy metals in surface seawater (Lao et al., 2019;
Wang et al., 2018; Zhang et al., 2015; Zhang et al., 2020), dynamics
(Monteiro and Roychoudhury, 2005; Tan et al., 2022) and chemical
speciation (Li et al., 2014; Wang et al., 2016a) of the dissolved heavy
metals in marine sediments or organisms (Hao et al., 2019; Lu et al.,
2017), partition between seawater and sediment (Liu et al., 2021; Wang
and Liu, 2003; Yuan et al., 2021) or SPM (Feng et al., 2017; Zhang et al.,
2018). However, there were less research on the dissolved heavy metals
in seawaters (Yin et al., 2015) compared to the extensive work in sedi­
ments and organisms in the YRE (Wang et al., 2016a; Wang et al., 2015;
Wang et al., 2014). The spatiotemporal comparison of dissolved heavy
metals distribution between surface and bottom seawater considering
the complex influencing factors in the YRE was even lacking. This limits
our understanding of the biogeochemistry of dissolved heavy metals in
the ocean and their interactions with the oceanic environmental
changes. Therefore, this study systematically investigated Cu, Pb, Cd,
As, and Zn, as well as the water properties in the surface and bottom
seawater off the YRE, East China Sea in order to: (1) analyze the
spatiotemporal distribution of dissolved heavy metals; (2) discuss
sources and the driving factors for the spatiotemporal distribution; (3)
assess the extent and risk of heavy metal pollution in seawater of this
region.
2. Materials and methods
2.1. Sample collection and seawater pretreatment
Three campaigns were carried out in spring (April), summer (July)
and autumn (September to October), 2019 off the YRE, East China Sea
on R.V. ZHEHAIHUANJIAN. Surface water samples were collected from
all the 66 stations, and bottom water samples were collected when water
depth was larger than 10 m using acid-cleaned GO-FLO sampler (Gen­
eral Oceanics) (Fig. 1). Onboard analysis included temperature (T) and
salinity (S) of the seawater by a salinometer (YSI30, USA), pH mea­
surement by a pH meter (Satorious PB-21, Germany) and dissolved ox­
ygen (DO) determined by dissolved oxygen meter (YSI 5100, USA).
About 100 mL surface and bottom seawater were filtered through a
pre-weighted cellulose acetate membrane onboard. The filter
Yangtze
River
East China Sea
Fig. 1. Map off Yangtze River Estuary and sampling sites (YRE-Yangtze River Estuary, HZB-Hangzhou Bay, XSH-Xiangshan Harbor, SMB-Sanmen Bay, YQB-
Yueqing Bay).
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Marine Pollution Bulletin 182 (2022) 113975
membranes were stored at − 20 ◦ C until lab analysis for SPM content. 2
mL magnesium carbonate suspension (10 g/L) was added to 50–1000
mL seawater and immediately filtered through a cellulose acetate
membrane onboard. The filter membranes were stored at − 20 ◦ C until
chlorophyll a (Chl a) analysis. About 400 mL of seawater was collected
using clean plastic bottles without filtration and were stored at − 20 ◦ C
until analysis for chemical oxygen demand (COD).
About 500 mL seawater was filtered through cellulose acetate filters
(0.45 μm, 47 mm diameter) immediately using a reusable bottle top
filter (Nalgene, USA). Then 100 mL filtrate in clean plastic bottles was
acidified to pH < 2 with sulfuric acid for As. Another 100 mL collected in
clean plastic bottles was acidified with nitric acid for Cu, Pb, Cd and Zn
analysis. The remaining filtrate were collected by precleaned plastic
bottles and frozen at − 20 ◦ C for nutrients. Bottles used for heavy metals
were soaked in nitric acid for one day and then rinsed with ultrapure
Milli-Q (Millipore, Bedford, MA, USA) water.
2.2. Environmental parameters and nutrients analysis
The filter membranes for SPM content were freeze-dried and
weighted in laboratory. The concentration of SPM retained on the
membrane was thus calculated. The filter membranes for Chl a mea­
surement was extracted with 90 % acetone. The extracts were deter­
mined using a spectrophotometer (TU1901, China) at wavelength of
664 nm, 647 nm, 630 nm and 750 nm. The relative standard deviations
for replicate analyses were < 10 %.
Nutrients including nitrate and soluble reactive phosphate (SRP)
were determined using a continuous flowing analyzer (SEAL AA3,
Germany). Seawater certified reference materials of GBW08631–08635
are used for the accuracy check. The relative standard deviations for
replicate analyses were < 5 %.
The COD was determined by alkalescent permanganate titration
method according to the specification for marine monitoring (Part 4:
seawater analysis) (GB 17378.4–2007) (General Administration of
Quality Supervision Inspection and Quarantine, 2008).
YRE
HZB
XSH
SMB
YQB
East China Sea
X. Hu et al.
2.3. Heavy metal determination and quality assurance
Preconcentration and separation of Cu, Pb, Cd, and Zn from the
seawater matrix were achieved using the ESI SP3 preconcentration
system (EPA 200.10) (U.S. Environmental Protection Agency, 1997).
The analytes were subsequently eluted into a simplified matrix con­
sisting of dilute nitric acid and were determined by ICP-MS (Perki­
nElmer, Nexion-300D, USA) using a directly coupled on-line
configuration. The standard solutions for calibrations were made with
five concentrations obtained by diluting a commercial standard multi­
element reagent (PerkinElmer, USA) with deionized water.
The concentration of As was determined using an atomic fluores­
cence spectrophotometer (AFS-9230, China) (General Administration of
Quality Supervision Inspection and Quarantine, 2008).
The determination limits were 0.050 μg⋅L− 1 for Cu, 0.003 μg⋅L− 1 for
Pb, 0.005 μg⋅L− 1 for Cd, 0.10 μg⋅L− 1 for As and 0.100 μg⋅L− 1 for Zn
respectively.
Seawater certified reference materials of CASS-6, NASS-7 and
GBW080040 are used for the accuracy check. The relative standard
deviations for replicate analyses were < 10 % and the recovery of
analysis varied from 80 % to 110 %.
The criteria value of the seawater quality standards of China (GB
3097–1997, China), and the reference table of Criteria Maximum Con­
centration (CMC) and Criteria Continuous Concentration (CCC) recom­
mended by the National Oceanic and Atmospheric Administration
(NOAA) (Buchman, 2008) were applied to evaluate the pollution status.
2.4. Statistical analysis
The spatial distribution maps were constructed using Ocean Data
View 4 (http://odv.awi.de, 2014). The hierarchical cluster analysis and
the heat map of the analytical results were plotted with dendrogram
using OriginPro 2021. The correlations among heavy metals, and be­
tween heavy metals and environmental parameters were statistically
analyzed by one-way analysis of variance (ANOVA). Principal compo­
nent analysis (PCA) and Pearson correlation analysis (CA) between
heavy metals and environmental parameters were carried out using
OriginPro 2021. The significance was determined when p < 0.05.
3. Results
3.1. Environmental parameters of the seawater
The average T (◦ C) (Table S1, S2; Fig. S1–1) followed a decreasing
order of summer (27.2 ± 1.4 ◦ C, 23.9 ± 2.1 ◦ C) > autumn (23.8 ±
1.7 ◦ C, 23.8 ± 1.6 ◦ C) > spring (16.2 ± 1.2 ◦ C, 15.8 ± 1.3 ◦ C) for surface
and bottom seawater, respectively. A cold-water mass showed in the
nearshore between XSH and SMB in spring. The T (◦ C) also decreased
from nearshore to offshore at the bottom seawater in summer. The T (◦ C)
at surface was higher than that at bottom in spring and summer but close
to the bottom water indicating mixed seawater in autumn.
The S varied from 0.2 to 33.3 and increased offshore (Table S2,
Fig. S1–2). Lower S was observed at surface in spring and summer
indicating the influence from Changjiang Diluted Water. The SPM was
higher in the YRE and HZB due to the river input and stronger sediment
resuspension at shallower depths (Table S2, Fig. S1–3).
The DO was higher in the offshore area at surface in summer
(Table S2, Fig. S1–4). On the contrary, the low DO was observed in the
offshore region located in the hypoxic zone of the YRE (Wei et al., 2007;
Wei et al., 2015) especially for bottom water in spring and summer. The
pH was higher in the east area at surface and lower in northeast area at
bottom in summer (Fig. S1–5), which was coincided with DO concen­
tration. The higher concentration of Chl a (Fig. S1–6) in the northeast
areas in spring and summer at surface corresponded with higher DO was
due to photosynthetic production.
Significant differences of environmental parameters (T, S, SPM, DO,
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Marine Pollution Bulletin 182 (2022) 113975
pH, Chl a) were observed between surface and bottom layer (ANOVA; p
< 0.05 for T and SPM and p < 0.01 for the other parameters). The
seasonal differences of T and DO were significant (ANOVA; p < 0.01) at
surface and bottom layer, and the S, SPM, pH, and Chl a concentration
was significant (ANOVA; p < 0.05 for SPM and p < 0.01 for the other
parameters) at surface layer (Table S1), suggesting obvious spatiotem­
poral features of environmental factors off the YRE.
3.2. Spatiotemporal distribution of dissolved heavy metals in seawater
The average concentrations of the dissolved heavy metals followed
similar patterns that in surface seawater, which followed a decreasing
order of As > Zn > Cu > Pb > Cd in spring, As > Cu > Zn > Pb > Cd in
summer and autumn, and in bottom seawater, which also followed the
decreasing order of As > Zn > Cu > Pb > Cd in spring and summer, and
As > Cu > Zn > Pb > Cd in autumn, respectively (Table S3, Fig. S2).
High values of the Cu concentration were observed in YRE and HZB
in spring and summer, and southwest near YQB in autumn (Fig. S2–1).
Spatial distribution of Pb indicated spread sites with higher concentra­
tion (Fig. S2–2), suggesting non-point sources from atmospheric depo­
sition. High values of Cd concentration (Fig. S2–3) could be observed
near YRE and YQB in spring (0.05 ± 0.01 μg⋅L− 1, 0.04 ± 0.004 μg⋅L− 1,
respectively) and autumn (0.06 ± 0.01 μg⋅L− 1, 0.06 ± 0.001 μg⋅L− 1,
respectively) for surface water, and in HZB and southern nearshore areas
in spring (0.04 ± 0.004 μg⋅L− 1, 0.04 ± 0.009 μg⋅L− 1, respectively) and
autumn (0.05 ± 0.001 μg⋅L− 1, 0.05 ± 0.007 μg⋅L− 1, respectively) at
bottom water. The As showed a downward trend from the estuary (2.00
± 0.74 μg⋅L− 1) to the offshore (1.63 ± 0.68 μg⋅L− 1) (Fig. S2–4). The
mean concentration of As followed a decreasing order in autumn >
summer > spring. The average concentration of Zn was 0.33 ± 0.34
μg⋅L− 1 for surface and 0.42 ± 0.72 μg⋅L− 1 for bottom water (Fig. S2–5).
The surface water showed higher Zn in YRE (0.69 ± 0.31 μg⋅L− 1) and
HZB (0.69 ± 0.44 μg⋅L− 1) in spring. Higher Zn was also observed in the
bottom water in YRE, HZB and YQB in spring with site ZJ0918 (6.44
μg⋅L− 1) and SH3114 (5.29 μg⋅L− 1) showing the highest in summer.
The concentration ratios between surface and bottom water were
compared. Spatially, about half of the samples showed ratios above 1.0
for Cu, Pb, Cd and As suggesting enrichment of these metals in the
surface water than the bottom water. Most samples had ratios lower
than 1.0 for Zn indicating enrichment of Zn in the bottom. Temporally,
all heavy metals in autumn in most samples showed ratios above 1.0
indicating surface enrichment likely due to water stratification effect
from late summer. In contrast, no specific patterns were observed in
spring and summer.
The results also suggested that all the samples were in good condition
within Grade I level of the seawater quality standard of China (GB
3097–1997, China) and no heavy metals exceeded the criteria maximum
concentration criteria of NOAA (Table S3).
3.3. Statistical results of the analytical parameters
The spatial sites could be divided into three groups by the hierar­
chical cluster analysis (Fig. S3). The three groups were then projected in
Fig. 2 that sampling sites could be separated into three spatial zones with
significantly different characteristics of the environmental parameters:
estuary, nearshore, and offshore (Figs. 3 and 4, Table S4), which
generally followed the influence from the Changjiang Diluted Water, the
Zhejiang and Fujian coastal current, and Taiwan Warm Current,
respectively.
The average T, SPM, SRP, nitrate and COD in the surface waters were
generally decreasing from estuary to offshore zone in the sampling
seasons (Fig. 3). The opposite trend was observed for S, DO, pH and Chl a
in the sampling seasons. The bottom waters witnessed similar spatial
trends in average SPM, SRP, nitrate, COD, S and Chl a (Fig. 4). The T,
however, increased from estuary to offshore in spring, but decreased in
summer and autumn indicating intrusion of open ocean deep water
X. Hu et al.
Fig. 2. Cluster distribution of dissolved heavy metals in surface water and bottom water in the three sampling seasons. The spatial sites are divided into three zones:
estuary zone (black dots), nearshore (red dots), and offshore (blue dots) based on cluster analysis. (For interpretation of the references to colour in this figure legend,
the reader is referred to the web version of this article.)
(Lian et al., 2016). The DO concentration decreased from estuary to
offshore in spring and summer while increased in autumn. The pH value
increased from estuary to offshore in spring and autumn.
Box plots of dissolved heavy metals in surface water in the three
zones were shown in Fig. 5 and Table S5. At surface, the concentration
showed a decreasing trend from estuary to offshore for Cu, Cd, As, Zn in
spring, Cu, As in summer, and As in autumn, respectively, while the
concentration of Pb showed an increasing trend from estuary to offshore
in all the seasons. In bottom water (Fig. 6, Table S5), the concentrations
of Cu, Cd, Zn decreased from the estuary to the offshore in spring. In
summer and autumn, higher Cu and Cd were observed in nearshore than
the estuary and offshore zones. The concentrations of Pb increased from
estuary to the offshore zone in both summer and autumn.
Statistically, PCA elucidated the sources and potential factors of the
distribution of dissolved heavy metals (Fig. S4 and S5). The first two
components of PCA explained 50 to 75 % of the total data variances. PC1
exhibited positive loadings for SRP and nitrate and negative loadings for
S in estuary indicating the influence from freshwater discharge. PC2
exhibited positive loadings for DO, pH and Chl a especially in summer in
the three zones suggesting effects from biological activities. For
example, in the estuary of the surface water, PC1 accounted for 34.1 %,
43.6 % and 40.6 % of the variance and exhibited significant positive
loadings for SRP and nitrate and negative loadings for salinity in spring,
summer and autumn, respectively (Fig. S4: a, d, g). These results indi­
cated the terrestrial influence. PC2 accounted for 17.0 %, 23.8 % and
19.8 % of the variance and exhibited high positive loadings for Cu, Pb,
As in spring, and positive loadings for DO, pH and Chl a in summer and
positive loadings for temperature in autumn. In the offshore of the
bottom water, PC1 accounted for 38.0 %, 29.2 % and 37.3 % of the
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Marine Pollution Bulletin 182 (2022) 113975
variance (Fig. S5: c, f, i) and exhibited negative loadings for salinity in all
the seasons and positive loadings for SPM in spring and summer. PC2
accounted for 17.4 %, 24.2 % and 26.0 % of the variance (Fig. S5: c, f, i)
and exhibited positive loadings for pH in all the seasons and exhibited
negative loadings for SPM in spring and autumn.
The correlation coefficients presented the extent of linear correlation
among dissolved heavy metals and environmental parameters (Figs. 7,
8). While the concentrations of Zn, Cd, As, Cu were generally correlated
(Figs. 7, 8), T, S, pH, and DO affect the distribution of different heavy
metals on different spatial and temporal scales. For instance, in the
surface water of the estuary, T exhibited significant positive correlations
with As in the three seasons (Fig. 7: a, d, g), but negative correlation with
Cd and Zn in summer. In the nearshore and offshore region, S exhibited
significant negative correlations with Cu and Cd in spring and autumn
(Fig. 7: b, c, i), and with Cu in summer (Fig. 7: e, f). The pH exhibited
significant negative correlations with Cd in summer (Fig. 7: e, f), and
with Cu and Zn in autumn (Fig. 7h), respectively. DO exhibited signif­
icant negative correlations with Cd in autumn (Fig. 7h). In the bottom
water, S significantly correlated with Pb negatively in spring in the es­
tuary (Fig. 8a) but positively in autumn in the nearshore (Fig. 8h). In the
estuary SPM positively affected the concentration of Cu, Pb, As and Zn in
summer (Fig. 8d), but negatively affected Cu and Zn in autumn in the
nearshore region (Fig. 8h). In autumn, DO and As were positively
correlated significantly in the estuary (Fig. 8g) but negatively correlated
in the offshore (Fig. 8i). The pH effect on Pb were temporally different
that they were negatively correlated in summer (Fig. 8e), while posi­
tively correlated in autumn (Fig. 8h) for the nearshore sites. In the
bottom of offshore sites, T negatively correlated with Cu and Cd in
spring and autumn (Fig. 8c, i), and positively correlated with As in
X. Hu et al.
Fig. 3. Box plots of environmental parameters in surface water in the three zones in spring, summer and autumn.
autumn. The Chl a exhibited significant positive correlation with Zn in
summer (Fig. 8f).
4. Discussion
4.1. Source effect on the distribution of dissolved heavy metals
The significant positive correlation among concentrations of Zn, Cd,
As, Cu (Figs. 7 and 8), indicated either identical sources or their similar
geochemical behavior (Kucuksezgin et al., 2008). In general, similar
sources were from terrestrial input by the Yangtze River that their
concentrations decreased from estuary to offshore zone (Figs. 5 and 6)
(Yin et al., 2015), accompanying by different geochemical behaviors
(see 4.4).
Zn has been reported to be mainly derived from wastewater from
river discharge (Cao et al., 2015). Temporally, decreased river discharge
in autumn reduced the Zn in estuary than that in nearshore. In the es­
tuary zone, the concentration of Zn showed a significant negative cor­
relation to DO and pH, which were similar to the results found in
Guangdong coastal waters (Zhang et al., 2015), Zhanjiang Bay (Zhang
et al., 2018), Beibu Gulf (Lao et al., 2019) and Meishan Bay (Zhang et al.,
2020), indicating that DO and pH would affect the Zn dynamics, eg.
biosorption of metal ions (Atkinson et al., 2007) in the ocean.
The wastewater discharge contain high levels of Cd (An et al., 2010)
which was possible sources of Cd to the ocean. The linear relationship
between Cd and SRP existed for the 28 surface samples in offshore
waters in summer that Cd (ng⋅L− 1) = 25.22 × SRP (μmol⋅L− 1) + 8.4, r =
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Marine Pollution Bulletin 182 (2022) 113975
0.89 (N = 26, p < 0.01). The slope was lower than that of northwest
Pacific Ocean (Matsunaga and Abe, 1985), and the molar ratio of Cd to
SRP (Cd/SRP = 2.3 × 10− 4) was half of those in plankton (4.9 × 10− 4)
(Bruland et al., 1978) due to overloading of phosphate in offshore of the
Yangtze River Estuary (Wang et al., 2012a), pointing out the close
relationship between Cd and SRP. The negative correlation between Cd
and SPM (r = − 0.26, p = 0.16) in spring in the estuary zone suggested
the adsorption effect on SPM. The complexation with chloride ions
(Garnier and Guieu, 2003) and pH (Wan et al., 2008a; Zhang et al.,
2017a) also greatly affected the Cd distribution (Fig. S4 and S5).
The projection of As and SPM was on the same principal component
in spring and summer. A negative correlation between As and S (r =
− 0.49, p < 0.01) and positive correlation between As and nitrate (r =
0.51, p < 0.01) (Fig. 7a, d) suggested the main source of As was from the
terrestrial input, such as application of arsenic contained pesticides in
crops (Sun et al., 2012). In the estuary zone, As showed a negative
correlation with other heavy metals in summer indicating different
geochemical behavior (Fig. 7d).
Pb has been suggested to mainly originate from petroleum producing
regions (Yang et al., 2015) showing no significant seasonal differences
(p > 0.05, Table S1) suggesting atmospheric deposition of exhaust gas
from anthropogenic sources (e.g. heavy traffic) (Wang et al., 2013;
Zhang et al., 2015). Particulates had minor effect on the distribution of
dissolved Pb in the estuary zone that no significant correlation was
found between Pb and SPM (Fig. 7: a, d, g). However, in the nearshore
the significant negative correlations between dissolved Pb and SPM
(Fig. 7: b, h) may suggest high availability of SPM adsorption surfaces to
X. Hu et al.
Fig. 4. Box plots of environmental parameters in bottom water in three zones in spring, summer and autumn.
dissolved Pb. As a result, with decreasing SPM offshore, the concentra­
tion of dissolved Pb increased from estuary to offshore, and higher
values in surface seawater was also observed than in the bottom
seawater (Fig. 5, Table S1).
4.2. Hydrodynamic and resuspension effects on the distribution of
dissolved heavy metals
The heavy metal distribution was affected not only by the sources but
also by the hydrodynamic factors (Wang et al., 2012b). Significant
different dissolved heavy metal concentrations (e.g. Cd, As, Zn) were
observed among seasons (ANOVA; p < 0.01, Table S1), suggesting
obvious temporal changes of dissolved heavy metals due to seasonal
hydrodynamic fluctuations of river discharge in Changjiang Diluted
Water.
The Changjiang Diluted Water spreads northeastward in summer
with the southwest monsoon and spreads southward in late fall to early
spring when the northeast monsoon prevails (Chen et al., 2021; Kwon
et al., 2018). Enhanced summer discharge enhanced SPM that the dis­
solved metals were easier to be scavenged through partitioning onto
solid particles, therefore the dissolved metals decreased seaward (Zhang
et al., 2008). For example, when the river flow decreased in spring and
autumn at the estuary, the larger SPM settled with finer SPM left. These
fine SPM always have large specific surfaces causing a high amount of
metals to be adsorbed (Wang et al., 2016b). So, the positive correlation
between Cd and SPM existed. When the river water mixed with
seawater, desorption processes usually appeared. But it seemed that the
desorption was not more important than the settling of SPM in river
water. Higher S would also lead to more Cd accumulation on SPM (Feng
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Marine Pollution Bulletin 182 (2022) 113975
et al., 2017; Liu et al., 2019b; Yin et al., 2015) that the complexation of
Cd2+ by chloride ions increased with the increasing S (Garnier and
Guieu, 2003). This resulted in the reduction of partition coefficient (KD)
of Cd (Turner et al., 2004). Therefore, Cd was desorbed with the salt­
water intrusion (i.e. concentration of Cd increased with the increasing S)
that the Cd speciation shifted easily towards dissolved CdCl+, CdCl2,
CdCl-3 and CdCl2-4 forms in seawater (Helmke, 1999). The positive cor­
relation between Cd and S found in estuary in summer and autumn could
be explained using this mechanism. Like Pb, Cu and Zn, the dissolved As
decreased seaward with increasing S indicating hydrodynamic effect.
Resuspension is an important mechanism for releasing metals into
the water column (Kalnejais et al., 2007) due to shear stress imposed by
hydrodynamics such as tidal currents (Bruland et al., 2008). The average
concentration of As and Zn in bottom water was higher than that in
surface water in summer in most zones (Table S5). This could be due to
sediment resuspension and weak vertical mixing in summer. Marine
sediments provided an excellent trap of anthropogenic impacts and
acted as source/sink for metals (Kang et al., 2017; Wang et al., 2017).
The summer water stratification hampered such mixing of higher bot­
tom resuspended heavy metals with surface water (Zhu et al., 2022).
Excessive releasement of dissolved heavy metals to the water column are
common during sediment resuspension such as in Mediterranean eco­
systems (Bancon-Montigny et al., 2019; Layglon et al., 2022), Portmán
Bay, Southern Spain (Bourrin et al., 2021), and lab simulated resus­
pension experiment (Burgess and Kester, 2002).
4.3. Biological effects on the distribution of dissolved heavy metals
The Chl a is commonly used as an indicator for phytoplankton
X. Hu et al. Marine Pollution Bulletin 182 (2022) 113975

Fig. 5. Box plots of dissolved heavy metals in surface water in three zones in spring, summer and autumn (unit: μg/L).

Fig. 6. Box plots of dissolved heavy metals in bottom water in three zones in spring, summer and autumn (unit: μg/L).

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X. Hu et al. Marine Pollution Bulletin 182 (2022) 113975

Fig. 7. Heatmap of Pearson correlations between heavy metals and environmental parameters in surface seawater in the three zones in spring, summer and autumn.

Fig. 8. Heatmap of Pearson correlations between heavy metals and environmental parameters in bottom seawater in the three zones in spring, summer and autumn.

biomass in the ocean. During the study period, the Chl a was higher in summer and autumn (Fig. 7: c, f, i) indicating the biological effects on
offshore in spring and summer at surface (Fig. 3), and it exhibited a the distribution of these heavy metals. Similarly, the negative correla­
negative correlation with Cd in spring and a positive correlation with As tion between Cu, Pb, Cd, Zn and Chl a existed (Fig. 7f) indicating

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X. Hu et al. Marine Pollution Bulletin 182 (2022) 113975

negative influence from biological processes. For instance, as nutrient-
type metals, dissolved Zn, Cd could be consumed by phytoplankton.
The decreased concentration of SPM in the estuary (Figs. 3 and 4)
resulted in increased transparency and intense biological activities
which led to phytoplankton assimilation of Zn thus the decreased Zn in
spring (Fig. 5). However, in coastal environments, the external inputs
(terrestrial, anthropogenic, sedimentary) of heavy metals have been
recognized to play the most important role than the hydrographic and
biogenic processes (Gavriil and Angelidis, 2005).
4.4. Pollution assessment of dissolved heavy metals and its feedback to
environmental change
Comparatively (Table 1), the average concentrations of Cu, Pb, Zn
and Cd in surface seawater were lower than the other regions in China
such as Northern Liaodong Bay, Jinzhou Bay, Yellow River Estuary and
Laizhou Bay. As was lower than that in the Pearl River Estuary and
higher than the Yellow River Estuary and Beibu Gulf, but close to
Laizhou Bay in spring. Pb, As and Zn were higher than that in Medi­
terranean Sea coast in Egypt. The average concentration of Cu, Pb, Cd
and Zn were higher than that in Saronikos Gulf in Greece and Tyrrhenian
coast in Italy. In any case, the investigation suggested that the water
belong to Grade I which fit the marine fishery, marine natural reserves as
well as rare and endangered marine protected areas, and no heavy
metals exceeded the CMC criteria of NOAA, indicating low ecological
risks of dissolved heavy metals in seawater off YRE (Table S3).
Environmental changes likely change the status of the dissolved
heavy metals in the water column. In the estuary (Fig. 7g), the dissolved
heavy metals showed positive correlation among each other and all were
negatively correlated with DO in the autumn, supporting the effects of
oxygen level on their distribution. In the nearshore (Fig. 7), the influ­
encing factors were complicated. The negative correlation between Cu,
Cd and S indicated the source effect in summer. Cd and As were
significantly correlated with T (Fig. 7g) indicating that a higher tem­
perature seemed to help their desorption from SPM. The negative cor­
relation between pH and Cu, Pb, Cd, Zn in autumn (Fig. 7h) indicated
the influence from potential acidification. In the offshore, the projection
of dissolved heavy metals in PCA was opposite to that of pH, indicating
that the dissolved heavy metals would increase with the decrease of pH
(Cu, Cd, Zn in spring; Cu, Pb, Zn, Cd in summer and Cu, Cd in autumn)
(Fig. S4: c, f, i). This indicates that pH played an important role that
ocean acidification would increase the concentration of some dissolved
heavy metals.

Table 1
Comparison of heavy metals concentration (μg⋅L− 1) in seawater with those in other regions.
Areas Period Cu Pb Cd As Zn Reference

Yangtze River Estuary Surface Spring, 2019 0.155–4.66 0.009–0.711 0.012–0.048 0.41–4.15 0.112–2.36 This study
0.465 ± 0.112 ± 0.033 ± 1.38 ± 0.60 0.541 ±
0.631 0.135 0.008 0.421
Yangtze River Estuary Surface Summer, 0.073–1.42 0.003–0.618 ND ~ 0.043 0.74–5.05 ND ~ 1.16 This study
2019 0.285 ± 0.077 ± 0.016 ± 1.96 ± 0.93 0.266 ±
0.266 0.130 0.010 0.270
Yangtze River Estuary Surface Autumn, ND ~ 1.89 ND ~ 0.423 0.009–0.071 0.99–4.69 ND ~ 0.904 This study
2019 0.398 ± 0.064 ± 0.031 ± 2.33 ± 0.61 0.182 ±
0.358 0.084 0.015 0.176
Yangtze River Estuary Bottom Spring, 2019 0.113–1.84 0.005–0.840 0.017–0.048 0.61–3.65 ND ~ 1.54 This study
0.301 ± 0.078 ± 0.031 ± 1.33 ± 0.45 0.461 ±
0.288 0.142 0.008 0.323
Yangtze River Estuary Bottom Summer, ND ~ 1.31 0.004–0.317 0.005–0.038 1.08–4.91 ND ~ 6.44 This study
2019 0.263 ± 0.058 ± 0.017 ± 1.80 ± 0.68 0.630 ± 1.19
0.265 0.064 0.009
Yangtze River Estuary Bottom Autumn, ND ~ 0.818 ND ~ 0.115 0.007–0.053 0.82–4.52 ND ~ 0.435 This study
2019 0.299 ± 0.037 ± 0.026 ± 2.19 ± 0.79 0.180 ±
0.210 0.030 0.012 0.099
Northern Liaodong Bay 2009(average) 2.86 3.98 0.66 5.46 17.76 (Zhang et al., 2017a)
Northern Liaodong Bay 2009(range) 0.70–6.20 0.60–17.20 0.10–1.40 1.92–10.10 1.20–82.80 (Zhang et al., 2017a)
Northern Liaodong Bay 2001–2005 4.34 3.21 0.995 NA 31.54 (Wan et al., 2008b)
Jinzhou Bay 2006 2.89 1.16 1.98 NA 30.46 (Wan et al., 2008a)
Jinzhou Bay 2009 3.06 0.61 0.92 2.19 11.87 (Wang et al., 2012b)
Bohai Bay 1996–2005 3.22 4.43 0.20 NA 43.92 (Mao et al., 2009)
Bohai Bay 1996–2005 16.30 40.40 0.89 NA 422 (Dai et al., 2009)
Bohai Bay 2007–2012 0.16–7.17 0.17–9.55 0.02–0.68 0.25–4.02 17.30–90 (Peng, 2015)
Yellow River Estuary 2009 2.65 0.51 0.68 0.92 NA (Tang et al., 2010)
Laizhou Bay 2010 15.88 0.88 0.28 1.40 NA (Lü et al., 2015)
East Guangdong coastal area, 2006–2007 2.24 1.94 0.11 2.48 14.05 (Zhang et al., 2015)
China
West Guangdong coastal area, 2006–2007 1.91 1.81 0.09 1.86 11.86 (Zhang et al., 2015)
China
Zhanjiang Bay 2014 4.40 0.23 0.12 NA 12.64 (Zhang et al., 2018)
Beibu Gulf, China 2003 1.08 0.74 0.07 1.24 NA (Lao et al., 2019)
Beibu Gulf, China 2017 3.03 0.71 0.17 0.74 10.0 (Lao et al., 2019)
The Pearl Estuary, China 1.64 1.61 0.12 2.55 13.54 (Zhang et al., 2013)
Deer Island,China 2010–2011 4.16 0.72 0.45 1.02 5.88 (Zhao et al., 2013)
Saronikos Gulf, Greece 2000–2001 2.80 2.85 0.32 NA 4.21 (Ladakis et al., 2007)
Tyrrhenian coast, Italy 2005 2.76 0.26 0.13 NA 9.32 (Manfra and Accornero,
2005)
Mediterranean coastal 2008 1.55 3.14 0.03 NA NA (Rossi and Jamet, 2008)
Mediterranean Sea coast, Egypt 2015 NA 0.006 NA 0.30 0.013 (El-Sorogy and Attiah,
2015)
North-western Bay of Bengal, 2010–2011 NA 1.39 0.01–0.30 NA 0.10–3.55 (Srichandan et al., 2016)
India
Belgian coastal zone 2010 3 0.14 0.21 NA 12 (Gao et al., 2013)

NA: not available.

9
X. Hu et al.
5. Conclusions
The average concentration of heavy metals was the highest for As,
followed by Cu or Zn, Pb, Cd. The distribution of the dissolved heavy
metals showed significant spatial and temporal variations off the YRE,
East China Sea. Spatially, the distribution of concentration was related
to pollutants sources either from continental land discharge, sediment
resuspension or atmospheric deposition. Temporally, significant differ­
ences on dissolved heavy metal concentrations were related to seasonal
hydrodynamic fluctuations. The principal component analysis and cor­
relation analysis showed that the spatial sites could be divided to three
zones: estuary, nearshore and offshore, which were affected by different
environmental factors such as DO, T, and pH etc. The concentration of
heavy metals suggested that all the samples were in good condition
within Grade I level of the seawater quality standard of China. The
physicochemical changes such as hypoxia, ocean acidification, global
warming along the estuary-nearshore-offshore zone would influence the
transportation, behavior and the bioavailability of the dissolved heavy
metals in marine environment and need more time series investigation
in the future.
Author statement
Conceptualization: XH, XS, XL.
Methodology: XH, XL.
Investigation: XH, XS, RS, YJ, SR, XL.
Visualization: XH, XL.
Funding acquisition: XS, XL.
Supervision: XS, XL.
Writing – original draft: XH, XL.
Writing – review & editing: XH, XS, RS, YJ, SR, XL.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Supplemental dataset
Acknowledgements
This work was supported by the Southern Marine Science and En­
gineering Guangdong Laboratory (Guangzhou) (GML2019ZD0210,
K19313901), Open Research Subject of Zhejiang Key Laboratory of
Petrochemical Environmental Pollution Control (2021Y04).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.marpolbul.2022.113975.
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