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Environmental Forensics

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Characteristics of heavy metals and persistentorganic pollutants in PM2.5 in two typical industrialcities, North China

Xixiang Yin, Guolan Fan, Jianjun Liu, Tenglong Jiang & Lihong Wang

To cite this article: Xixiang Yin, Guolan Fan, Jianjun Liu, Tenglong Jiang & Lihong Wang (2020):Characteristics of heavy metals and persistent organic pollutants in PM2.5 in two typical industrialcities, North China, Environmental Forensics, DOI: 10.1080/15275922.2020.1771635

To link to this article: https://doi.org/10.1080/15275922.2020.1771635

Published online: 13 Jun 2020.

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Characteristics of heavy metals and persistent organic pollutants in PM2.5 intwo typical industrial cities, North China

Xixiang Yina, Guolan Fana, Jianjun Liua, Tenglong Jianga, and Lihong Wangb

aWater-Soil Research Section, Jinan Eco-environmental Monitoring Center, Jinan, China; bShandong Analysis and Test Centre, QiluUniversity of Technology (Shandong Academy of Sciences), Jinan, China

ABSTRACTWe collected PM2.5 samples in the cities of Jinan and Baotou, North China. Concentrationsof 9 heavy metals (HMs) (Cr, As, Cd, Sb, Pb, Ni, Cu, Zn, Mn) and 2 persistent organic pollu-tants [polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and dioxin-like poly-chlorinated biphenyls, (DL-PCBs)] (POPs), were determined. The concentrations of PM2.5-bound HMs exhibited apparent seasonal characteristics in both cities. In Jinan, the highestlevels of As, Cd, Sb, Pb, Cu, Zn occurred in the heating season, while, the levels of Cr, Ni,Mn peaked in the windy season. In Baotou, The order of concentrations of HMs in PM2.5

was as follows: heating season> non-heating season>windy season. In both cities, theheating season had the highest concentrations of 17 PCDD/Fs and 12 DL-PCBs. Only a smallamount of them occurred in the windy season. In Baotou, RPCDD/Fs and RDL-PCBs levelswere much higher than in Jinan, except in the non-heating season. The health risk of car-cinogenic metal concentrations for adults was approximately twice than that for children.Notably, the Cr risk for adults slightly exceeded the critical value in Baotou.

KEYWORDSPM2.5; heavy metals; POPs;health risk; China

1. Introduction

In recent years, owing to rapid urbanization and mas-sive energy consumption, haze events occur more fre-quently in many areas of China and it is nowgenerally acknowledged that atmospheric pollution isbecoming a significant environmental problem (Huet al., 2014). Air particulate matter, especially fine par-ticles (PM2.5) appears to be strongly associated withthe deterioration of air quality by light extinction(Tao et al., 2014; Jiang et al., 2019; Li et al., 2019).Meanwhile, numerous studies have demonstrated thatPM2.5 is also harmful to human health (Moreno et al.,2007; Brook et al., 2010; Thurston et al., 2016). Leiliet al. (2008) reported that lung diseases and otherorganic damage resulting from atmospheric heavymetals have been well-documented. It is noteworthythat the rate of premature deaths caused throughPM2.5 exposure in China is more than 1,300,000 peo-ple annually (Liu et al., 2016).

Fine particles (PM2.5) are the preferential carrierfor many elements or metals, due to their greater sur-face area, even for toxic heavy metals and persistentorganic pollutants such as PCDD/Fs and DL-PCBs,

(Chi et al., 2009; Lu et al., 2009; Bi et al., 2020).Generally, PM2.5 toxicity rests on its chemical com-position. Naturally derived toxic substances are usuallyfound in coarse particles (Stone et al., 2011), however,those of anthropogenic origin are mainly distributedin fine particles which can carry more toxic chemicalsto human beings and ecosystems, than the coarse frac-tions (Fang et al., 2009; Chen et al., 2010; Zhaoet al., 2011).

Jinan is the capital of Shandong province in theeast China, and close to the south of Tai Mountainand north of the Yellow River. It is a typical coal-based energy resource consumption city. Baotou is thelargest city in Inner Mongolia, and is also known asone of the most industrialized cities of northwestChina. In the past decade, due to energy structure,industrial layout and adverse diffusion conditions,haze episodes have occurred frequently over the twocities and their peripheral regions (Yang et al., 2013;Gu et al., 2014; Li et al., 2016). Previous studies havemainly focused on PM2.5 concentration and elementalcomposition in some megacities and their key airquality control areas (Xie et al., 2019; Wu et al.,2019a; 2019b). To our knowledge, for typical

CONTACT Lihong Wang wlhkxy@163.com Shandong Analysis and Test Centre, Qilu University of Technology (Shandong Academy of Sciences),Jinan, 250014, China� 2020 Informa UK Limited, trading as Taylor & Francis Group

ENVIRONMENTAL FORENSICShttps://doi.org/10.1080/15275922.2020.1771635

industrial cities, the study of seasonal characteristicsof PM2.5-bound toxic chemicals and relevant healthrisk assessments has seldom been addressed.

Here, we collected PM2.5 samples in Jinan andBaotou to analyze the accumulation, distribution andseasonal variation in PM2.5 heavy metals and persist-ent organic pollutants, and to assess the correspond-ing exposure health risks.

2. Materials and methods

2.1. Sampling

Sampling sites (117.062269 E, 36.669194N; 109.872905E, 40.674793N) were located on the roofs of theEnvironmental Monitoring Center (EMC) (about 17mabove the ground) in Jinan and Baotou, respectively(Figure 1). Eighteen-hour (18 h) PM2.5 samples (8:30a.m. to 2:30 a.m. the next day) were collected in threetypical seasons (windy season: May 6-21, 2011; non-heating season: October 8-22, 2011; heating season:December 6-20, 2011) on prebaked (780 �C, 3 h) quartzfilters (90mm, Munktell Ahlstrom, Falun, Sweden) in aparticulate sampler (TH-150S, Wuhan TianhongInstrument Co., Ltd, Wuhan, China) with a flow rateof 100 L min�1. Before and after sampling, the filterswere equilibrated for 24h in a chamber with a constanttemperature (�23 �C) and relative humidity (�50%),and then weighted with an electronic microbalance(FA1004, Lichen, China). All samples were finallysealed in a clean filter container (100mm) and pre-served in a refrigerator (-18 �C) until analysis.

2.2. Analysis of heavy metals

A quarter of each sample filter was cut into piecesand then dissolved in mixtures of HNO3 (9ml, 65%)and HClO4 (3ml, 70%). After a 24 h digestion, thesolution was boiled, the residue was dissolved with10ml of 6.5% HNO3 and then diluted in a 25ml flaskwith ultrapure water. The diluted solutions weretransferred to numbered polyethylene vials and storedin a refrigerator (4 �C) for subsequent analysis. Theconcentrations of Cr, As, Cd, Sb, Pb, Ni, Cu, Zn, andMn were determined by an ICP-MS (7500a AgilentTechnologies).

2.3. Determination of organic toxic substances

The target compounds were 17 PCDD/Fs and 12 DL-PCBs. For the purposes of this paper, we refer to thesums of the corresponding compounds as RPAHs(excluding retene, listed separately as marker of wood

combustion), RPCDD/Fs and RDL-PCBs. QFFs wereextracted with toluene using an automatic extractor(BUCHI Extraction System B-811, Switzerland). C-13labeled compounds were spiked onto each QFF beforeextraction. The extracts were concentrated using anitrogen stream. Samples were transferred to a silicacolumn followed by a carbon column for PCDD/Fsand DL-PCBs. PCDD/Fs and DL-PCBs were analyzedusing a 7890A gas chromatograph (GC) (Agilent,USA) equipped with a 60m [ 0.25mm [ 0.25mmDB5-MS column (Agilent J&W, USA) coupled to anAutoSpec Premier high resolution mass selectivedetector (GC-HRMS) (Waters, Micromass, UK). TheHRMS was operated in electron impact ionization(EIþmode) at a resolution of >10,000. PAHs wereanalyzed using a 6890 GC (Agilent, USA), equippedwith the same column as mentioned above, coupledto a mass selective detector (MS 5975, Agilent USA)(Holoubek et al., 2007).

2.4. Health risk assessments

2.4.1. Exposure assessmentHealth risks caused by PM2.5 heavy metals were calcu-lated on the basis of inhalation of fine particlesthrough the respiratory pathway. Pollutants can bedivided into non-carcinogens and carcinogens accord-ing to United States Environmental Protection Agency(EPA). Hence, Pb, Zn, Cu, Mn, Sb were classified asnon-carcinogenic, while As, Cd, Cr, Ni were classifiedas carcinogenic. We used a classical assessment modelrecommended by the EPA to evaluate health risk(EPA, 1989). For carcinogens, the lifetime averagedaily dose (LADD, mg kg�1 day �1) via inhalation iscommonly used for the assessment of cancer risk,while the normal average daily dose (ADD, mgkg�1 day �1) is used for non-carcinogens. The equa-tion is as follows:

ADD=LADD ¼ Cp� FP � IR� EDBW � AT

(1)

Where Cp stands for the PM2.5 concentration (kgm�3), FP is the concentration of a certain element(mg kg�1), ED is the exposure duration (day), BW isbody weight (kg), and AT is average exposure time(day). The values of these parameters were summar-ized in Table 1.

2.4.2. Risk characterization of heavy metals in PM2.5

The annual excess risk (R) was calculated based onexposure dose to evaluate the risks of carcinogens(Rc) and non-carcinogens (Rt) caused by airbornemetals. The formulae are as follows:

2 X. YIN ET AL.

Rc ¼ ð1� e�LADD�SFÞ=70 (2)

Rt ¼ ADD� 10�6=ðRfD� 70Þ (3)

Where SF is the slope factor (mg kg�1 d�1), 70 isthe average life expectancy (year), and RfD is the ref-erence dose of inhalation path (mg kg�1 d�1) (Table2). A risk of less than 10�6 is an internationallyacceptable threshold value.

2.5. Quality assurance and quality control

Given the accuracy and precision, certified referencesample (GSB 04 1767-2004, National Analysis andTesting Center, China) was used for heavy metals ana-lysis. The range of recoveries for all heavy metals wasbetween 90.6% and 112.7%. Blanks (including filters)and duplicate samples were analyzed for approxi-mately 10% of the samples.

For quality control of PCDD/Fs and DL-PCBs, alaboratory blank and matrix spike sample were ana-lyzed after every eight samples. Blank levels of indi-vidual analytes were in most cases below detectionand very low otherwise (on average less than 1.5% ofsample mass for all compounds). Method detectionlimits (0.02–0.10 fg m�3) were determined from theblanks and quantified at three times the standarddeviation of the concentration in the blanks. All quan-tities reported here have been corrected for blanks.Recovery efficiency ranged from 63% to 108% forPCDD/Fs and DL-PCBs, respectively.

2.6. Statistical analysis

Principal Component Analysis (PCA), using uncon-strained ordination analysis in Canoco 5, was utilizedto investigate the relationships between heavy metals,

organic pollutants and PM2.5. The PM2.5 heavy metalconcentration data was analyzed using analysis ofvariance (ANOVA).

3. Results and discussion

3.1. Characteristics of heavy metals bound withPM2.5 in Jinan and Baotou

The average PM2.5 concentrations in Jinan were 2.1,2.3 and 3.6 times higher than National Ambient AirQuality Standard of China (35 mg/m3, GB 3095-2012,Class I) in three periods, respectively (Figure 2).Notably, PM2.5 levels were far higher than 75 mg/m3

(GB 3095-2012, Class II) in more than 96% of sam-pling days, and the maximum reached 162 mg/m3. InBaotou, the PM2.5 concentration range was from56.3� 94.5 mg/m3, which was significantly lower thanin Jinan. However, they still were up to 1.6, 1.9 and2.7 times higher than Class I, respectively. Moreover,the PM2.5 mass concentrations in different periods inboth cities were in descending order: heating season->non-heating season>windy season. Notably, PM2.5

levels in Jinan were relatively high, compared withother cities (Wang et al., 2006; 2013; Tan et al., 2014;Gao et al., 2018). Although the models of fuel con-sumption have always been changing as result ofindustrial restructuring in Jinan, coal is still the pri-mary fuel and is used extensively for industrialmanufacturing and daily life, especially in the central-heating season. Coal consumption for heating only ismore than 2 million tons per year in Jinan, and isprobably the main reason for high PM2.5 levels inwinter in this city.

The PM2.5 heavy metal concentrations were alsodetermined and showed a highly seasonal pattern inJinan (Figure 2A). The highest As, Cd, Sb, Pb, Cu,and Zn concentrations occurred in the heating season,and were 6.71 ng/m3, 1.37 ng/m3, 3.22 ng/m3, 76.08 ng/m3, 11.11 ng/m3, and 127.18 ng/m3, respectively. Thewindy season had the lowest concentrations of2.76 ng/m3, 0.32 ng/m3, 1.16 ng/m3, 25.7 ng/m3,9.64 ng/m3, and 76.02 ng/m3, respectively. Meanwhile,the remaining three heavy metals (Cr, Ni, Mn)reached maximum values of 6.28 ng/m3, 4.07 ng/m3,and 54.04 ng/m3, respectively, in the windy season. Crand Mn had their lowest concentrations (4.21 ng/m3,

Table 2. The parameters of dose-reaction from theinhale approach.Elements Characterization SF [mg/(kg�d)] RfD [mg/(kg�d)] Sources

As carcinogen 20.07 EPACd carcinogen 8.4 HEACr carcinogen 56 HEANi carcinogen 1.19 HEAPb non-carcinogen 4.3� 10�4 HEAZn non-carcinogen 1.0� 10�2 HEACu non-carcinogen 2.0� 10�3 HEAMn non-carcinogen 3.0� 10�4 HEASb non-carcinogen 　 8.6� 10�4 WHO

Table 1. The exposure parameters of the inhale approach.Population IR (m3/d） BW (kg) ED (d) AT (d) carcinogens AT (d) non-carcinogens

Adults (male) 19.2 70 30� 365 70� 365 30� 365Adults (female) 14.17 60 30� 365 70� 365 30� 365Children 5.65 36 18� 365 70� 365 18� 365

ENVIRONMENTAL FORENSICS 3

18.4 ng/m3) in the non-heating season, while, the min-imum Ni concentration was during the heating sea-son. Seasonal heavy metal patterns in Baotou weresomewhat different to those in Jinan. The nine PM2.5

heavy metal concentrations over three periods inBaotou were in descending order: heating season->non-heating season>windy season (Figure 2B).The maximum concentrations reached 22.46 ng/m3,

6.96 ng/m3, 1.65 ng/m3, 3.66 ng/m3, 165.37 ng/m3,7.74 ng/m3, 47.4 ng/m3, 329.61 ng/m3, and 299.19 ng/m3, respectively. Zheng et al. (2018) showed thatheavy metal levels in aerosols usually showed seasonalvariation and followed the order: winter> autumn> -spring> summer. Furthermore, heavy metal levelswere lowest in summer, probably due to high frequentprecipitation and flourishing vegetation. High concen-trations of PM2.5-bound heavy metals frequentlyoccurred in the heating season, likely due to the staticand stable meteorological conditions and anthropo-genic discharge, especially from coal heating in winterin North China (Cao et al., 2012). Meanwhile, heavymetal levels were higher in Jinan than in Baotou inwindy seasons, except Cr, Cu and Mn. The mass con-centrations of six heavy metals (Cr, As, Cd, Sb, Pb,Ni) in Jinan were similar to those in Baotou duringthe non-heating season, but remarkably, Cu, Zn, andMn concentrations in Baotou were much higher thanthose in Jinan. Furthermore, Cr, Pb, Ni, Cu, Zn andMn concentrations in Baotou, far exceeded those inJinan in the heating season.

It was clear that Zn, Pb and Mn were the mostabundant metals in PM2.5 (Figure 3). Commonly, Znis considered as a traffic and industrial elementaltracer (Liu et al., 2017). In our study, it was enrichedin PM2.5, indicating that traffic and industrial sourceemissions contributed greatly to the pollution of fineparticulates. After the prohibition of leaded gasolinein China in1997, coal combustion has become the

Figure 1. The locations of sampling sites in two cities. Source: Authors.

Figure 2. The concentrations of PM2.5 at three seasons in twotypical cities.

4 X. YIN ET AL.

main Pb emission source in airborne particulate mat-ter. Based on data from China Statistical Yearbooks,annual coal consumption in Jinan and Baotouaccounted for c. 0.6% and 1.1%, respectively, of totalcoal consumption in China in 2011. Previous studiesreported that Mn was the major pollutant in soil androad dust, especially in Asian natural soil dust(Manoli et al., 2002; Chang et al., 2009; Lim et al.,2010; Lee et al., 2011). Given the rapid urbanizationof the two cities over the last decade, the enforcementof environmental management should be strength-ened. Overall, by comparison with other cities, suchas Shanghai, Guangzhou, X�ıan and Tianjin, the metalconcentrations associated with PM2.5, especially Cr,As, Cd and Pb, were low in Jinan and Baotou (Wanget al., 2006; Lu et al., 2008; Zhai et al., 2014; Chenet al., 2015).

To better understand the accumulation and distri-bution of PM2.5 heavy metals for the two cities,PM2.5/PM10 concentration ratios of nine heavy metalswere analyzed in Figure 4. PM2.5/PM10 mass concen-tration ratios for nine heavy metals were mostly >

50% in Jinan, except in the heating season (Figure3A). As Lee and Hieu (2011) demonstrated, a largeproportion of heavy metals were mainly distributed inthe fine particles. The situation was totally different inBaotou, where PM2.5/PM10 ratios were > 50% only inthe heating season (Figure 3B). Obviously, highPM2.5/PM10 ratios signify that PM10 is mainly com-posed of fine particles (PM2.5). In this study, it is clear

that heavy metals accumulate more in PM2.5, ratherthan in PM2.5-10 in Jinan throughout the samplingperiod. It is well known that the PM2.5 accumulationrate is associated with the extent of industrial activitiesand traffic intensity, which can result in the increasedhealth risks caused by heavy metals (Srishti et al.,2017). Unlike Jinan, heavy metals are more likely toexist in PM2.5-10, indicating that the correspondinghealth risks may be generated by relatively coarse par-ticulates in Baotou.

3.2. Characteristics of PM2.5 organic pollutants inthe two cities

The total concentrations of PCDD/Fs and DL-PCBs inPM2.5 were determined for three seasons in the twocities (Figure 5). The highest PCDD/Fs concentrationsof 227.9 and 391.7 fg I-TEQ m�3 were found duringthe heating season in Jinan and Baotou. Meanwhile,the lowest concentrations occurred in the windy sea-son, which were only 39.7 and 66.4 fg I-TEQ m�3,respectively. Previous studies confirmed that the mainPCDD/Fs emission sources are from fossil fuel com-bustion and certain industrial activities (e.g. metalsmelting processes and waste incineration; Chen et al.,2018). Consequently, mass consumption of coal forheating in winter is responsible for the situation.

Given their high lipophilicity, toxicity and degrad-ation difficulty, DL-PCBs are viewed as typical persist-ent organic pollutants (Guo et al., 2014; Liu et al.,

Figure 3. The concentrations of nine heavy metals in PM2.5 in Jinan (A) and Baotou (B) at three typical seasons.

ENVIRONMENTAL FORENSICS 5

2014). In our study, in contrast to that observed withRPCDD/Fs, the city concentrations of RDL-PCBs inPM2.5 indicated some similar seasonal tendency. Theheating season had the highest concentrations of DL-PCBs, up to 21.1 and 14.6 fg I-TEQ m�3, respectively,in Jinan and Baotou. Only a small amount of DL-PCBs (0.74 fg I-TEQ m�3 in Jinan and 3.46 fg I-TEQm�3 in Baotou) occurred during the windy season.Coal fly ashes (CFAs) are a known PCBs emissionsource in the literature (Li et al., 2016). Our data alsosuggested that DL-PCBs values were much higher inwinter than in the other two periods, which can beexplained by more coal consumption for winter heat-ing, especially in North China.

Notably, as shown in Figure 5, the levels of PCDD/Fs and 12 DL-PCBs in Baotou were much higher thanin Jinan except in the non-heating season, which maybe explained by higher coal consumption and adversemeteorological conditions in Jinan. Additionally, com-bined with the levels of PM2.5 shown in Figure 2, theroughly negative correlations between the levels ofPM2.5 and PCDD/Fs and 12 DL-PCBs can be observedexcept in the non-heating season.

Besides, as seen in Figure 6, the results of Principalcomponent analysis (PCA) between heavy metals,organic pollutants and PM2.5 in two cities wereshown. Obviously, the concentrations of PM2.5 had apositive correlation with the levels of heavy metals

Figure 4. The PM2.5/PM10 ratios of heavy metal concentrations in typical seasons in Jinan (A) and Baotou (B).

Figure 5. The concentrations of PCDD/Fs (A) and DL-PCBs (B) bound with PM2.5 at typical seasons in Jinan and Baotou.

6 X. YIN ET AL.

and organic pollutants in the heating season, whichwas very similar in both cities. However, little correl-ation of the three can be observed in other two sea-sons. It can suggest that the significant increase offossil energy consumption may cause the rising con-centrations of pollutants in PM2.5. Some additionalstudies have recorded the similar conclusions (Yinet al., 2017; Chen et al., 2018).

3.3. Health risk assessments of PM2.5-boundtoxic pollutants

To further assess the potential threat to local residentscaused by PM2.5 heavy metals, the average annualexcess risks (Rc: carcinogen risk; Rt: non-carcinogenrisk) for adults and children using the inhalationapproach were evaluated using the US EPA assess-ment model. The parameters of exposure and dailydose-reaction are listed in Tables 1 and 2. In Jinan, Rc

values for four carcinogenic elements were in the fol-lowing order: Cr>As>Cd>Ni (Table 3).Additionally, there were substantial differencesbetween age groups, for example, the risks caused byPM2.5-bound metals for adults were close to 2 timesthat of children, indicating that adults may be morevulnerable than children, although all risks were belowthe threshold value (1[10�6). Meanwhile, the risks forfive noncarcinogenic elements for adults and childrenwere both within the safe range and ranked in theorder: Mn> Sb>Zn> Pb>Cu. Compared to Jinan,two differences were notable in Baotou (Table 4).Firstly, the risk of Cr for adults slightly exceeded the

critical value, showing the adults might face a Cr-caused cancer risk in Baotou. Secondly, the AS Rcvalue for children was nearly twice that for adults,which suggests that greater attention should be paidto how to control it, even though it was still withinthe safe limit. Because of the lack of PCDD/Fs andDL-PCBs data, the health risk caused by organic toxicpollutants could not be analyzed.

4. Conclusions

In 2 Chinese cities, PM2.5 concentrations were investi-gated, and 9 types of heavy metals (HMs) (Cr, As, Cd,Sb, Pb, Ni, Cu, Zn, Mn) were analyzed to ascertaintheir seasonal variation and potential effects onhuman health. The highest PM2.5 concentrationsoccurred in the heating season, followed by the non-heating season and windy season, successively. ThePM2.5 heavy metal concentrations varied seasonally inthe two cities. In Baotou, the levels of RPCDD/Fs andRDL-PCBs were higher than in Jinan except in thenon-heating season. Furthermore, the underlying car-cinogenic and non-carcinogenic risks caused by HMswere investigated. In Jinan, Rc values for four carcino-genic elements were in the following order:Cr>As>Cd>Ni. The health risks of PM2.5 carcino-genic elements for adults were about twice as high asfor children. The Cr for adults slightly exceeded thecritical value in Baotou, indicating it may pose apotential health risk.

Figure 6. Principal component analysis (PCA) between heavymetals, organic pollutants and PM2.5 in Jinan and Baotou.

Table 3. The average annual excess risks of heavy metals inJinan for various populations.Elements Adults (male) Adults (female) Children

Cr (10�7) 5.92 5.15 2.05As (10�8) 17.0 14.7 5.88Cd (10�9) 11.5 10.0 3.99Ni (10�9) 5.37 4.67 1.86Sb (10�10) 2.60 2.26 1.50Mn (10�10) 5.31 4.61 3.07Pb (10�11) 3.87 3.36 2.23Cu (10�11) 2.33 2.02 1.35Zn (10�11) 4.42 3.84 2.55

Table 4. The average annual excess risks of heavy metals inBaotou for various populations.Elements Adults (male) Adults (female) Children

Cr (10�6) 1.37 1.19 0.48As (10�8) 1.28 1.11 4.43Cd (10�9) 12.5 10.8 4.32Ni (10�9) 3.88 3.37 1.35Sb (10�10) 3.60 3.13 2.08Pb (10�11) 5.39 4.68 3.11Cu (10�11) 9.02 7.84 5.21Zn (10�11) 8.89 7.72 5.13Mn (10�10) 19.2 16.7 11.1

ENVIRONMENTAL FORENSICS 7

Acknowledgements

We warmly thank Dr. Hongyu Xu for helping us samplecollection in this study. We also thank Dr. Xiaoyan Sun forassisting in sample analysis.

Funding

This study was financially supported by the NationalNatural Science Foundation of China (41671485),Distinguished Middle-Aged and Young Scientist Encourageand Reward Foundation of Shandong Province (CN)(BS2013HZ009), and Natural Science Foundation ofShandong Province (CN) (ZR2017MD008).

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