The environment quality of metals in surface sediments in Hangzhou Bay

doi:10.21203/rs.3.rs-4718582/v1

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The environment quality of metals in surface sediments in Hangzhou Bay

https://doi.org/10.21203/rs.3.rs-4718582/v1

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Hangzhou Bay is facing the environmental pressure brought by the economic development of the surrounding areas, but the comprehensive and systematic study of heavy metals in the sediments was still insufficient. In this study, heavy metals (Cu, Pb, Zn, Cr, Ni and V) in 231 surface sediments in Hangzhou Bay were analyzed to evaluate their spatial distribution and pollution status and their controlling factors. The contents of metals in sediments had a low level and were not facing serious ecological risk on the whole. However, most metals exhibited higher concentrations in the central and northeastern parts of Hangzhou Bay, while Zn and Cr showed elevated contents in the adjacent area of the Qiantang River mouth, where the environmental quality assessment of metals showed low-to-moderate pollution, which was worthy of attention. The heavy metals in the sediments were primarily from natural sources and their distribution was mainly dominated by the grain size of the sediments. However, Pb in the northern coastal areas and Cr and Zn in the Qiantang River mouth were found to have high contents and indicated relatively serious pollution potentially caused by human activities. This study is of great scientific significance for understanding the accumulation and source-sink process of heavy metals in the sediments of the Bay of intense human activities.

heavy metals

environment quality

surface sediment

Hangzhou Bay

Bays are important areas of land-sea interaction and are the most active areas of human activities, which act as interfaces between continents and open seas and buffer zones to filter contaminants (Costanza et al., 1997; Tian et al., 2022). With the development of economy and society, an increasing number of environmental problems have arisen in the semi-enclosed bays from anthropogenic activities and their ecosystems were under great pressure, including the pollution of heavy metals in the sediments (Özkaynak et al., 2022; Guan et al., 2024). Thus, it is of great significance to study the heavy metals in the sediments of bays, while their spatial distributions in the sediments could provide basic information for determining the environmental health risks (Peng, 2015; Xu et al., 2016; Tian et al., 2022).

Heavy metals in the sediments carried by rivers into the sea, which come from natural processes of weathering and erosion, as well as various anthropogenic sources such as industrial and agriculture activities, sewage disposal, and so on, were mostly deposited in estuaries and bays and had an important impact on aquatic ecological environment (Xu et al., 2017). On the one hand, heavy metals in sediments migrate between liquid and solid phases via water–sediment exchange reaction, which affects the aquatic environmental quality; on the other hand, most heavy metals are nondegradable toxic substances, and the accumulation of ecological effects lead to the absorption and enrichment by organisms in the food chain, eventually causing chronic poisoning (Vicente-Martorell et al., 2009; Achary et al., 2016; Liu et al., 2019). Different sources and influencing factors control metals contamination at different spatial scales, and identifying the spatial variations could reveal the sources and environmental health status of metals within bay sediments (Zhao et al., 2015; Jafarabadi et al., 2017). In recent years, many studies focused on the environmental quality of sediment in bays and evaluated the pollution status of heavy metals in sediments, revealed that many areas have experienced serious heavy metal pollution (Liu et al., 2022; Tang et al., 2022; Tong et al., 2023; Guan et al., 2024).

Hangzhou Bay is located in the eastern coastal area of China, adjacent to the Yangtze River Estuary in the north and the East China Sea in the east, covering an area of approximately 8,500 km² (Liu et al., 2012). It is a typical funnel-shaped estuary with strong tide, rapid flow, and high sediment content (Wu et al., 2011). Alluvial plains were widely distributed on the north and south banks of Hangzhou Bay, and the underlying layers of the loose sediments was mainly the sedimentary rocks, however, the sediments in Hangzhou Bay mainly come from the Yangtze River, followed by the Qiantang River which influence area was limited to the southern part of the bay, and the influence of coastal erosion materials can be basically ignored (Che et al., 2003; Liu et al., 2012; Wang et al., 2013). With the continuous economic and social development in the basin of Yangtze River, Qiantang River and the surrounding areas of Hangzhou Bay in recent years, intensified the transport of terrestrial source pollutants and has an important impact on the ecological environment of Hangzhou Bay (Zhang et al., 2002; Che et al., 2003; Zhang et al., 2008; Pang et al., 2015; Fang et al., 2016; Bao et al., 2021). However, previous studies were mostly confined to the local area of Hangzhou Bay. Thus, this study aimed to illustrate the spatial distribution and assess the pollution status of the heavy metals (Cu, Pb, Zn, Cr, Ni, and V) in the whole area of Hangzhou Bay. Furthermore, it aimed to provide valuable information on the environmental quality of these heavy metals in sediments in Hangzhou Bay through comprehensive and systematic research.

2.1 Study area and sampling

A total of 231 surface sediment samples were collected from Hangzhou Bay during a large-scale sedimentological investigation cruise from April to May 2008 (Fig. 1). The upper 5 cm of the sediments was sampled using a plastic scoop at each site for grain size and elemental analysis. All samples were placed in polyethylene bags and stored in a refrigerator at 4°C before analysis.

2.2 Methods

2.2.1 Grain size analysis

The grain size of sediment samples was measured using Malvern Mastersizer 2000 at the Key Laboratory of Marine Sedimentology and Environmental Geology, State Oceanic Administration, China. Before analysis, the samples were preprocessed using 30% H₂O₂ and 1-mol/L HCl solutions to decompose organic matter and carbonate, respectively. The mean grain size (Mz) of the sediments was calculated using the Matrix method (McManus, 1988). The repeat-test relative errors were < 2%.

2.2.2 Heavy metal concentration analysis

The samples were dried and ground to a 63-µm particle size, followed by digestion of 0.05-g sample using a mixture of HNO₃ and HF. The concentrations of SiO₂, Al₂O₃, as well as metals of Cu, Pb, Zn, Cr, Ni, and V were determined using an inductively coupled plasma optical emission spectrometer (Thermo Fisher Scientific iCAP6300). To ensure quality control and assurance, standard sediment samples GSD-9 and GSD-10 were analyzed alongside parallel samples. Statistical analysis revealed that the relative standard deviations for element analysis were below 5%.

The professional cartographic software Surfer16.0 was used to map the distribution of geochemical elements contents and the heavy metal environmental quality assessment results in this study.

2.2.3 Pollution status assessment methods

Geo-accumulation index (I_geo)

The geo-accumulation index (I_geo), originally defined by Müller (1969), is a widely used parameter to assess heavy metal contamination. The I_geo values are defined by the formula below:

I _geo =log₂($\:\frac{{C}_{i}}{1.5{B}_{i}}$) (1)

where C_i is the measured content of an metal, and B_i is the geochemical background concentration of the metal; the value 1.5 is a background matrix correction factor that includes possible variations in the background values due to lithogenic effects (Müller, 1969). In this study, the elemental content of sedimentary rocks (mainly shale) in the global lithosphere (Li, 1990) were used as the background metal values B_i, and the background values were 40 mg/kg, 15 mg/kg, 90 mg/kg, 72 mg/kg, 56 mg/kg, and 63 mg/kg for Cu, Pb, Zn, Cr, Ni, and V, respectively. A seven levels classification of the I_geo is defined as: unpolluted (I_geo ≤ 0); unpolluted to moderately polluted (0 < I_geo ≤ 1); moderately polluted (1 < I_geo ≤ 2); moderately to strongly polluted (2 < I_geo ≤ 3); strongly polluted (3 < I_geo ≤ 4); strongly to extremely polluted (4 < I_geo ≤ 5); and extremely polluted (I_geo > 5) (Müller, 1969).

Potential ecological hazard index

The potential ecological hazard index proposed by Hakanson (Hakanson, 1980) was used to assess the ecological risk of a single heavy metal and the total amount of heavy metals. The calculation formulas of single factor index and comprehensive pollution index are as follows:

C _f = C_i/B_i (2)

C _d =$\:\:{\sum\:}_{i=1}^{n}{C}_{f}^{i}$ (3)

where C_f is the pollution index of the single heavy metal, C_i is the measured concentration of the heavy metal in the sediments of each sample, and B_i is the geochemical background concentration of the metal, here we also used the elemental content of sedimentary rocks in the global lithosphere; C_d is the comprehensive pollution index of all the heavy metals in sediments.

$$\:{E}_{r}={T}_{r}^{i}\times\:{C}_{f}^{i}={T}_{r}^{i}\frac{{C}_{i}}{{B}_{i}}$$

$$\:{E}_{RI}=\sum\:_{i=1}^{n}{E}_{r}^{i}$$

where E_r is the single potential ecological hazard index of heavy metal; $\:{T}_{r}^{i}$is the toxicity coefficient formulated according to the ecological activity of each heavy metal, and the toxicity coefficients of Cu, Pb, Zn, Cr, Ni and V are 5, 5, 1, 2, 5 and 2, respectively (Hakanson, 1980); $\:{E}_{RI}$ is the comprehensive potential ecological hazard index of various heavy metals in sediments (Hakanson, 1980). The degree of pollution is classified in the Table 1.

Table 1

The potential ecological risk assessment index and their relative pollution degree
C_f	Pollution degree of single factor	C_d	Overall pollution degree	E_r	Ecological harm degree of single factor	E_RI	Overall potential ecological risk degree
< 1	low	< 8	low	< 40	low	< 150	low
1 ~ 3	moderate	8 ~ 16	moderate	40 ~ 80	moderate	150 ~ 300	moderate
3 ~ 6	heavy	16 ~ 32	heavy	80 ~ 160	Moderate-heavy	300 ~ 600	heavy
≥6	serious	≥32	serious	160 ~ 320	heavy	≥600	serious
				≥320	serious

3.1 Distributions of heavy metals in surface sediment

The distribution patterns of the mean grain size (Mz) and SiO₂, Al₂O₃, Cu, Pb, Zn, Ni, and V are presented in Fig. 2. The Mz of the surface sediments greatly varied, ranging from 5.60 to 137.39 µm, with the mean value of 16.53 µm. Fine-grained sediments such as clay and fine silt mainly covered the northern, central, and eastern parts of Hangzhou Bay (Fig. 2). Coarse silt and sand were distributed off the Qiantang River mouth and extended further to the southeast of Hangzhou Bay, as well as some patchy area in the northeast and southeast of the study site.

The distribution of the SiO₂ content exhibited a striking resemblance to that of Mz, with an increase of approximately 50.0% in the northern, central, and eastern regions of Hangzhou Bay to around 70.0% near the Qiantang River mouth, suggesting its predominant enrichment in coarse-grained sediments. Contrarily, the Al₂O₃ content ranged above 13.5% in the sediments of central and northern parts of Hangzhou Bay but dropped as low as 10.0% at the Qiantang River mouth (Fig. 2), suggesting its primary enrichment in fine-grained sediments.

The content statistics of heavy metals are shown in Table 2. In general, the heavy metals, except Zn and Cr, tended to exhibit higher concentrations in the central and eastern parts of Hangzhou Bay and similar distribution patterns to Al₂O₃ while displaying lower concentrations in areas with coarser sediments such as the Qiantang River mouth. However, the distribution patterns of Zn and Cr differed from those of other elements, exhibiting elevated levels in the Qiantang River mouth or its southern adjacent area (Fig. 2). This finding suggests a distinct source and/or divergent sedimentary behaviors of different heavy metals.

Table 2

Summary of statistic analysis for contents and evaluation results in the surface sediments of Hangzhou Bay
		Cu		Pb	V	Zn	Ni	Cr
Contents of metals in sediments of Hangzhou Bay (mg/kg)	Minimum		4.71	1.73	56.06	49.12	18.32	47.79
	Maximum		50.71	62.38	154.10	230.83	61.96	150.91
	Average		31.11	23.04	112.36	97.54	40.32	79.76
Geo-accumulation index (I_geo)	Minimum		-3.67	-3.70	-1.27	-1.14	-2.20	-0.98
	Maximum		-0.24	1.47	0.19	1.10	-0.44	0.68
	Average		-1.05	-0.13	-0.29	-0.18	-1.09	-0.26
C_f	Minimum		0.12	0.12	0.62	0.68	0.33	0.76
	Maximum		1.27	4.16	1.71	3.21	1.11	2.40
	Average		0.78	1.54	1.25	1.35	0.72	1.27
E_r	Minimum	0.59		0.58	1.25	0.68	1.64	1.52
	Maximum	6.34		20.79	3.42	3.21	5.53	4.79
	Average	3.88		7.68	2.50	1.35	3.60	2.53

3.2 Pollution assessment of heavy metals in surface sediment

The total content of metals in the sediments is largely determined by the amount they occur naturally, the amount increased by human activities, and the ability of the sediment to hold metals introduced into the system (Mecray and Buchholtz Ten Brink, 2000). However, the total concentrations of heavy metals in the sediments do not represent the level of contamination (Zhou et al., 2007). Therefore, it is important to determine whether the contamination levels pose a threat to aquatic ecosystems. Many methods can be used to evaluate the pollution status of heavy metals in sediments (Turekian and Wedepohl, 1961; Forstner and Müller, 1973; MacDonald et al., 1996, 2000; Long et al., 1998; Nobi et al., 2010), with the geo-accumulation index and potential ecological hazard index being more widely used.

As shown in Table 2, the calculated values of I_geo in the surface sediments of Hangzhou Bay varied from − 3.67 to − 0.24 with an average of − 1.05 for Cu, − 3.70 to 1.47 with an average of − 0.13 for Pb, − 1.27 to 0.19 with an average of − 0.29 for V, − 1.14 to 1.10 with an average of − 0.18 for Zn, − 2.20 to − 0.44 with an average of − 1.09 for Ni, and − 0.98 to 0.68 with an average of − 0.26 for Cr. Obviously, the sediments in the central and northern parts of Hangzhou Bay exhibited higher I_geo values, which were influenced by the adsorption effect of fine sediments (Fig. 3).

The average I_geo value indicated that the surface sediments in Hangzhou Bay were unpolluted by heavy metals and that the mean pollution level of these metals decreased in the following order: Pb, Zn, Cr, V, Cu, and Ni. However, Pb, Zn, Cr, and V showed unpolluted to moderate or moderate contamination in some areas (Fig. 3), such as the northern part of Hangzhou Bay for Pb and V showed the highest pollution levels near a port outside the mouth of the Qiantang River, whereas Zn and Cr had the highest pollution level near the north and south banks of the Qiantang River estuary, respectively. The high level of heavy metal pollution in estuarine and coastal areas is definitely influenced by the pollutants produced by human activities.

As presented in Fig. 4, the distribution of the single-factor pollution index (C_f) of each metal is similar to that of I_geo. However, the average value of C_f indicated the moderate pollution status of Pb, Zn, Cr, and V (Table 2), whereas these elements show moderate pollution status in most study sites of Hangzhou Bay. The pollution levels of Cu and Ni were found to be relatively low, the overall pollution state at low level (Table 2), and only a few stations showed moderate pollution. The areas with high pollution levels were mainly distributed in the northern, central, and eastern parts of Hangzhou Bay, consistent with the distribution of sediment particle size, but those with the highest Zn and Cr pollution levels were in the Qiantang River estuary.

The comprehensive pollution index of six types of heavy metals in sediments (C_d) ranged from 2.84 to 10.99, with an average value of 6.86. Therefore, the overall pollution level was low, but in the central and northeastern parts of the study site, the pollution index was obviously greater than 8. However, the comprehensive pollution indicator (C_d) is affected by the number of heavy metals, and as the number of heavy metals involved in the assessment increases, the index also increases; thus, more attention should be paid to the spatial distribution of C_d rather than its specific value.

When the potential ecological hazard index of the surface sediments of Hangzhou Bay was evaluated, considering the ecotoxicity coefficient of heavy metals, the pollution status of heavy metals was different from those evaluated using previous methods. Pb remains to have the highest pollution level; however, Cu and Ni also had higher pollution levels than other metals. In this study, the E_r of the metals ranged from 0.59 to 6.34 for Cu (average 3.88), 0.58 to 20.79 for Pb (average 7.68), 1.25 to 3.42 for V (average 2.50), 0.68 to 3.21 for Zn (average 1.35), 1.64 to 5.53 for Ni (average 3.60), and 1.52 to 4.79 for Cr (average 2.53) (Table 2). The mean pollution level of the metals decreased in the following order: Pb > Cu > Ni > Cr > V > Zn. The ecological hazard index of heavy metals was generally considered to be low pollution, but serious pollution was observed in the central area of Hangzhou Bay. However, of particular note, most metals were found in the central and northern parts of the study site with high contamination levels, particularly in the coastal area of northern Hangzhou Bay. This highlights the need to strengthen the in-depth investigation of this element and its sources and take necessary measures to reduce or eliminate its potential threat to the environment.

According to the analysis, the comprehensive potential ecological hazard brought by six heavy metals was within the range of low-grade pollution. The E_RI values ranged from 6.52 to 38.81, with an average of 21.37, which was lesser than the threshold of low pollution level. However, some heavily polluted areas were observed in the central part and northern coastal area of Hangzhou Bay, indicating a potentially higher degree of environmental risk in the area; thus, corresponding measures need to be taken. The comprehensive pollution index is also subject to changes in the amounts of different types of heavy metals. Therefore, when assessing the ecological risks of metals, we need to consider the potential impacts of different types, quantities, and interactions on environmental health.

To explore the controlling factors influenced the heavy metals distribution in the surface sediments in Hangzhou Bay, Pearson’s correlation analysis and principal component analysis (PCA) on the contents of heavy metals, SiO₂ and Al₂O₃, as well as sediment grain size were conducted using the SPSS software (version 25). The results of correlation analysis (Tables 3) indicated a significant positive correlation between each heavy metal and Al₂O₃, reflecting their similar sources and migration behavior. However, a significant negative correlation was observed between their content and sediment grain size and SiO₂ concentration, whereas only a weak correlation was observed between Cr and grain size.

Table 3

Pearson’s correlation matrix for the heavy metals, SiO₂, Al₂O₃ and Mz.
	SiO₂	Al₂O₃	Cu	Pb	V	Zn	Co	Ni	Cr
Al₂O₃	-0.657^**
Cu	-0.936^**	0.626^**
Pb	-0.602^**	0.541^**	0.578^**
V	-0.901^**	0.627^**	0.838^**	0.492^**
Zn	-0.730^**	0.507^**	0.751^**	0.499^**	0.664^**
Co	-0.866^**	0.663^**	0.820^**	0.527^**	0.834^**	0.669^**
Ni	-0.931^**	0.651^**	0.892^**	0.523^**	0.890^**	0.719^**	0.848^**
Cr	-0.553^**	0.409^**	0.484^**	0.294^**	0.696^**	0.375^**	0.694^**	0.585^**
Mz	0.677^**	-0.504^**	-0.693^**	-0.421^**	-0.532^**	-0.461^**	-0.450^**	-0.633^**	-0.143^*
Note: ** Correlation is significant at the 0.01 level (2-tailed).

*Correlation is significant at the 0.05 level (2-tailed).

As presented in Table 4, two principal components were obtained via PCA. F1 accounted for 45% of the total variance, heavy metals and Al₂O₃ had significant loadings on this factor, whereas SiO₂ and Mz exhibited negative loadings. As a chemically inactive compound, Al₂O₃ was stable during the formation of sediments and was not influenced by the environment, which is often used as an indicator of terrestrial components in the ocean (Liu et al., 2019; Chaudhary et al., 2013). Previous studies have shown that the heavy metal pollution caused by human activities in Hangzhou Bay could not be distinguished and the seawater quality was in good condition (Zhang et al., 2008; Liu et al., 2012). Therefore, this factor indicated that the distribution of elements in the surface sediments in Hangzhou Bay was mainly influenced by sediment grain size and that the sediments were largely derived from the weathering of terrigenous materials.

The total variance contribution rate of F2 was determined to be 32%, with Cr and Mz identified as the main loading elements. The distribution pattern of Cr greatly differed from other elements, exhibiting higher concentrations in areas characterized by coarse sediments near the Qiantang River and Cao-e River estuary (Fig. 2). This discrepancy can be attributed to pollution caused by human activities. However, the Qiantang River, Cao-e River and Yong River, with more than 444.4×108 m3/a water discharged into the Hangzhou Bay, accounting for more than 30% of the total water discharge entering the Hangzhou Bay, may contribute significantly to heavy metals pollution in the vicinity of their estuaries, such as the highest Cr value can be found near Cao-e River Estuary (Zhang et al., 2002; Liu et al., 2012).

Table 4

Matrix of factor loadings of the heavy metals, SiO₂, Al₂O₃ and Mz.
Variable	Factor loading
Variable	F1	F2
SiO₂	− .965	.053
Al₂O₃	.753	− .097
Mz	− .666	.565
Cu	.937	− .133
Pb	.659	− .234
V	.916	.201
Zn	.772	− .111
Co	.902	.248
Ni	.943	.022
Cr	.616	.709
Percentage of total variance (%)	45.52	32.40

The assessment of the environmental quality of heavy metals using both the geological accumulation index (I_geo) and potential ecological hazard index (E_r) was based on the background value of heavy metals, and different pollution levels could be obtained with different background values (Rubio et al., 2000). I_geo mainly reflects the pollution and accumulation of heavy metals caused by human activities and considers diagenetic factors that may cause changes in background values (such as coefficient k) (Liu et al., 2015; Looi et al., 2019). However, E_r focuses on the toxic effects of various heavy metals at the biological level to determine the toxicity or risk of heavy metal pollutants to aquatic ecosystems (Hakanson, 1980). The results of the I_geo and E_r evaluation indicated that the heavy metals in the surface sediments of Hangzhou Bay did not exhibit high pollution levels. The heavy metals in the sediments are mainly from natural sources, and their distribution is mainly affected by the grain size of the sediments.

However, some heavy metals in the central and northern coastal areas of the study site and the area near the Qiantang River mouth showed a low-to-moderate pollution level. In the central and northern coastal areas of Hangzhou Bay, possibly due to the sediment contribution from the Changjiang River (Sheng et al., 2008; Sun et al., 2009), the Pb concentration and pollution level were much higher than the other area, close to the value of the Changjiang Estuary, which are ∼37 and ∼28 µg/g respectively (Sheng et al., 2008). In addition, Cr and Zn near the Qiantang River mouth and Cao-e River mouth which had higher contents, should come from the contribution of these rivers. So, the several heavy metals in the above areas are clearly significantly affected by human activities, which requires further attention.

The average contents of heavy metals Cu, Pb, Zn, Cr, Ni and V in the surface sediments of Hangzhou Bay were 31.11 mg/kg, 23.04 mg/kg, 97.54 mg/kg, 112.36 mg/kg, 40.32 mg/kg, and 79.76 mg/kg, respectively. The heavy metals except Zn and Cr tended to exhibit higher concentrations in the central and eastern parts of Hangzhou Bay, while Zn and Cr showed elevated levels in the Qiantang River mouth or its southern adjacent area.

The environmental quality assessment of metals indicated that the surface sediments in Hangzhou Bay were not facing serious ecological risk on the whole. However, Pb in the northern coastal areas and Cr and Zn in the Qiantang River mouth showed a low-to-moderate pollution level, which was worthy of attention.

The heavy metals in the sediments were primarily from natural sources and their distribution was mainly dominated by the grain size of the sediments. In areas with high heavy metal content and relatively serious pollution, the sources of heavy metals in sediments were affected by human activities. The heavy metals in sediments of central and northern coastal areas of Hangzhou Bay possibly influenced by the sediment contribution of Yangtze River, and that in the Qiantang River mouth and Cao-e River mouth impacted by the input from these rivers.

Author Contribution

Weifeng Liu, Shengfa Liu, Hui Zhang and Wei Jiang wrote the main manuscript text, Hui Zhang and Wei Jiang prepared figures 1-5. Shengfa Liu organized the survey and provided the sediment samples studied in the paper.

Acknowledgments

We thank staff from First Institute of Oceanography, Ministry of Natural Resources, China for sample collecting on board. This work was supported by Coastal Investigation and Research Project of China (908-01-CJ09, 908-ZC-I-05).

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No competing interests reported.

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The environment quality of metals in surface sediments in Hangzhou Bay

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Version 1

Abstract

Figures

1. Introdution

2. Materials and methods

2.1 Study area and sampling

2.2 Methods

2.2.1 Grain size analysis

2.2.2 Heavy metal concentration analysis

2.2.3 Pollution status assessment methods

3. Results

3.1 Distributions of heavy metals in surface sediment

3.2 Pollution assessment of heavy metals in surface sediment

4. Factors controlling the distribution of heavy metals

5. Conclusions

Declarations

Author Contribution

References

Additional Declarations

Status:

Version 1