南京北郊冬季PM2.5中重金属的形态、来源及健康风险

doi:10.19741/j.issn.1673-4831.2022.0335

摘要/Abstract

摘要： 为探究南京北郊冬季PM_2.5重金属的污染特征、来源与健康风险,于2021年1-2月采集PM_2.5样品,用BCR连续提取法对11种元素(Al、V、Cr、Mn、Co、Cu、As、Cd、Sr、Ba和Pb)进行连续提取,用电感耦合等离子体原子光谱仪(ICP-OES)测定分析PM_2.5中重金属的化学形态和分布特征,利用正定矩阵因子分解模型(PMF)解析其来源,采用基于生物可利用浓度修正的美国国家环境保护局(EPA)健康风险评价模型评估其健康风险,并结合PMF模型、浓度权重轨迹模型(CWT)和后向轨迹模型(HYSPLIT)对特定污染源和区域传输的影响进行评估。结果表明:(1)采样期间PM_2.5日均质量浓度为(99.0±18.3)μg·m^-3,采样期间有92.3%的天数超过GB 3095-2012《环境空气质量标准》日均浓度限值,11种元素的日均总质量浓度为(1 999.0±307.2)ng·m^-3,其中As、Cd日均质量浓度分别为(7.0±3.5)和(22.0±14.0)ng·m^-3,均高于GB 3095-2012标准限值。(2)大部分重金属(V、Cr、Mn、As、Sr、Cd、Ba)主要存在于生物可利用性极高的弱酸溶解态(F1),Co、Cu和Pb主要存在于可还原态(F2),Al主要存在于生物可利用性较低的残渣态(F4)。(3)利用PMF模型解析出3类排放源,分别是扬尘源(31.4%)、燃煤源(17.7%)、交通和工业混合源(50.9%)。(4)采样期间重金属的综合非致癌风险指数小于1,非致癌风险可忽略,Cr、Co、As、Cd有潜在致癌风险。结合PMF、CWT和HYSPLIT发现,交通和工业混和源及河南省信阳市和安徽省东部的区域传输对南京北郊健康风险的影响不容忽视,因此不仅要加强对本地工业源排放的管控,也要密切关注区域传输对本地的影响。

关键词: PM_2.5, 重金属, 生物可利用性, 来源解析, 特定源健康风险

Abstract: To explore the pollution characteristics, sources, and source-specific health risks of PM_2.5-bound heavy metals (HMs) during winter in the north suburb of Nanjing, daily PM_2.5 filter samples were collected during January and February 2021. The distribution characteristics and chemical speciation of 11 HMs (Al, V, Cr, Mn, Co, Cu, As, Sr, Cd, Ba and Pb) in PM_2.5 were determined by BCR extraction and ICP-OES. Positive matrix factorization (PMF), as well as the modified health risk assessment method was used to analyze the source-specific health risks of HMs, which could find out the major health abuser. The influence of the regional transmission was evaluated using PMF, the concentration-weighted trajectory (CWT) method and Hybrid Single Particle Lagrangian Integrated Trajectories (HYSPLIT), respectively. The results showed that the average daily concentration of PM_2.5 was (99.0±18.3) μg·m^-3, and 92.3% of the days in the sampling period exceeded the daily average limit of the National Ambient Air Quality Standard (GB 3095-2012). The total contents of HMs was (1 999.0±307.2) ng·m^-3, while the average value of As and Cd were (7.0±3.5) and (22.0±14.0) ng·m^-3 ,respectively,both higher than the GB 3095-2012 limit value. Most of the studied HMs (V, Cr, Mn, As, Sr, Cd, Ba) were mainly concentrated in acid-soluble fraction (F1) with high bioavailability, a relatively high percentage of Co, Cu and Pb were present in reducible fraction (F2). Al was mostly concentrated in residual fraction (F4) with low bioavailability. Dust sources (31.4%), coal sources (17.7%) and the mixed sources of traffic and industry (50.9%) were the main sources of metal elements. Non-cancer risks of heavy metals were negligible with values under 1, and Cr, Co, As, Cd posed potential cancer risk to child and adults with values between 10^-6 and 10^-4. It could not be ignored that the impact of the mixed sources of industrial and traffic and regional transmission from Xinyang city of Henan Province and eastern Anhui Province on health risks in the northern suburbs of Nanjing. Therefore, it is not only necessary to strengthen the control of local industrial emissions, but also to pay close attention to the impact of regional transmission.

Key words: PM_2.5, heavy metals, bioaccessibility, source apportionment, source-specific health risk

中图分类号:

X513

赵腾, 孙明洋, 盖鑫磊. 南京北郊冬季PM_2.5中重金属的形态、来源及健康风险[J]. 生态与农村环境学报, 2023, 39(10): 1257-1266.

ZHAO Teng, SUN Ming-yang, GE Xin-lei. Chemical Speciation, Source Appointment and Health Risk Assessment of Heavy Metals in PM_2.5 in Winter in the North Suburb of Nanjing[J]. Journal of Ecology and Rural Environment, 2023, 39(10): 1257-1266.

参考文献 32

[1]	MENG J H,SHI X F,XIANG Y,et al.Current Status and Sources of Heavy Metal in Atmosphere[J].Environmental Science and Management,2017,42(8):51-53.
[2]	WANG S S,HU G R,YU R L,et al.Bioaccessibility and Source-Specific Health Risk of Heavy Metals in PM2.5 in a Coastal City in China[J].Environmental Advances,2021,4:100047.
[3]	LI P H,YU J,BI C L,et al.Health Risk Assessment for Highway Toll Station Workers Exposed to PM2.5-bound Heavy Metals[J].Atmospheric Pollution Research,2019,10(4):1024-1030.
[4]	刘桓嘉,贾梦珂,刘永丽,等.新乡市大气PM2.5载带金属元素季节分布、来源特征与健康风险[J].环境科学,2021,42(9):4140-4150.[LIU Huan-jia,JIA Meng-ke,LIU Yong-li,et al.Seasonal Variation,Source Identification,and Health Risk of PM2.5-bound Metals in Xinxiang[J].Environmental Science,2021,42(9):4140-4150.]
[5]	钱新,王金花.南京大气PM2.5中重金属形态分布及健康风险[C]//第六届重金属污染防治及风险评价研讨会暨重金属污染防治专业委员会2016年学术年会论文集.厦门:[出版者不祥],2016:12-19.
[6]	代鹏飞,王帅,钱坤,等.某铀矿区农田土壤重金属生物有效性分析[J].生态与农村环境学报,2021,37(5):644-650.[DAI Peng-fei,WANG Shuai,QIAN Kun,et al.Analysis of Bioavailability of Heavy Metals in Farmland Soil in Uranium Mining Area[J].Journal of Ecology and Rural Environment,2021,37(5):644-650.]
[7]	韩存亮,罗炳圣,常春英,等.基于多种方法的区域农业土壤重金属污染成因分析研究[J].生态与农村环境学报,2022,38(2):176-183.[HAN Cun-liang,LUO Bing-sheng,CHANG Chun-ying,et al.Identifying the Source of Soil Heavy Metal Pollution in Regional Agricultural Area Based on Multiple Methods[J].Journal of Ecology and Rural Environment,2022,38(2):176-183.]
[8]	DAI Q L,LIU B S,BI X H,et al.Dispersion Normalized PMF Provides Insights into the Significant Changes in Source Contributions to PM2.5 after the COVID-19 Outbreak[J].Environmental Science & Technology,2020,54(16):9917-9927.
[9]	张晓雨,赵欣,应蓉蓉,等.广州大气PM2.5中含碳组分的污染特征及来源解析[J].生态与农村环境学报,2018,34(7):659-666.[ZHANG Xiao-yu,ZHAO Xin,YING Rong-rong,et al.Characteristics and Source Apportionments of Carbonaceous Components in Atmospheric Fine Particles in Guangzhou[J].Journal of Ecology and Rural Environment,2018,34(7):659-666.]
[10]	WANG J F,YU J,GONG Y,et al.Pollution Characteristics,Sources and Health Risk of Metals in Urban Dust from Different Functional Areas in Nanjing,China[J].Environmental Research,2021,201:111607.
[11]	徐蕾,肖昕,马玉,等.徐州农田土壤重金属空间分布及来源分析[J].生态与农村环境学报,2019,35(11):1453-1459.[XU Lei,XIAO Xin,MA Yu,et al.Sources and Spatial Distributions of Heavy Metals in Xuzhou Farmland Soils[J].Journal of Ecology and Rural Environment,2019,35(11):1453-1459.]
[12]	李慧明,钱新,冷湘梓,等.南京市PM2.5中金属元素污染特征及健康风险[J].环境监控与预警,2021,13(1):7-13.[LI Hui-ming,QIAN Xin,LENG Xiang-zi,et al.Pollution Characteristics and Health Risks of Metal Elements in PM2.5 from Nanjing[J].Environmental Monitoring and Forewarning,2021,13(1):7-13.]
[13]	TIAN S S,LIU Y Y,WANG J,et al.Chemical Compositions and Source Analysis of PM2.5 during Autumn and Winter in a Heavily Polluted City in China[J].Atmosphere,2020,11(4):336.
[14]	YANG B,ZHOU L L,XUE N D,et al.Source Apportionment of Polycyclic Aromatic Hydrocarbons in Soils of Huanghuai Plain,China:Comparison of Three Receptor Models[J].Science of the Total Environment,2013,443:31-39.
[15]	翟诗婷,王申博,张栋,等.郑州市典型污染过程PM1中重金属浓度、来源及健康风险评估[J].环境科学,2022,43(3):1180-1189.[ZHAI Shi-ting,WANG Shen-bo,ZHANG Dong,et al.Concentration,Source,and Health Risk Assessment of PM1 Heavy Metals in Typical Pollution Processes in Zhengzhou[J].Environmental Science,2022,43(3):1180-1189.]
[16]	LIU P P,LEI Y L,REN H R,et al.Seasonal Variation and Health Risk Assessment of Heavy Metals in PM2.5 during Winter and Summer over Xi'an,China[J].Atmosphere,2017,8(5):91.
[17]	任万辉,李云丹,苏枞枞,等.沈阳市大气PM2.5中重金属污染特征、来源解析及健康风险评价[J].环境化学,2021,40(4):1029-1037.[REN Wan-hui,LI Yun-dan,SU Cong-cong,et al.Pollution Characteristics,Source Apportionment and Health Risk Assessment of Heavy Metals in PM2.5 in Shenyang[J].Environmental Chemistry,2021,40(4):1029-1037.]
[18]	KERMANI M,JONIDIJAFARI A,GHOLAMI M,et al.Characterization,Possible Sources and Health Risk Assessment of PM2.5-Bound Heavy Metals in the Most Industrial City of Iran[J].Journal of Environmental Health Science and Engineering,2021,19(1):151-163.
[19]	LIU E F,WANG X Y,LIU H J,et al.Chemical Speciation,Pollution and Ecological Risk of Toxic Metals in Readily Washed off Road Dust in a Megacity (Nanjing),China[J].Ecotoxicology and Environmental Safety,2019,173:381-392.
[20]	XU H X,WANG Y,LIU R H,et al.Spatial Distribution,Chemical Speciation and Health Risk of Heavy Metals from Settled Dust in Qingdao Urban Area[J].Atmosphere,2019,10(2):73.
[21]	周燊港,邹海凤,董娴,等.贵阳市冬季PM2.5中典型重金属元素的化学形态分析与健康风险评价[J].生态毒理学报,2017,12(1):277-284.[ZHOU Shen-gang,ZOU Hai-feng,DONG Xian,et al.Chemical Speciation of Typical Heavy Metals and Health Risk Assessment in PM2.5 during Winter in Guiyang City[J].Asian Journal of Ecotoxicology,2017,12(1):277-284.]
[22]	魏复盛,陈静生,吴燕玉,等.中国土壤环境背景值研究[J].环境科学,1991,12(4):12-19,94.[WEI Fu-sheng,CHEN Jing-sheng,WU Yan-yu,et al.Study on the Background Contents on 61 Elements of Soils in China[J].Environmental Science,1991,12(4):12-19,94.]
[23]	姚森,王乾恒,薛妍,等.郑州市冬季大气PM2.5金属元素来源及健康风险评价[J].环境科学,2022,43(5):2329-2335.[YAO Sen,WANG Qian-heng,XUE Yan,et al.Source Apportionment and Health Risk Assessment of Metal Elements in Ambient PM2.5 in the Winter of Zhengzhou[J].Environmental Science,2022,43(5):2329-2335.]
[24]	周安琪,刘建伟,周旭,等.北京大气PM2.5载带金属浓度、来源及健康风险的城郊差异[J].环境科学,2021,42(6):2595-2603.[ZHOU An-qi,LIU Jian-wei,ZHOU Xu,et al.Concentrations,Sources,and Health Risks of PM2.5 Carrier Metals in the Beijing Urban Area and Suburbs[J].Environmental Science,2021,42(6):2595-2603.]
[25]	李星谕,毛瑶,陈展乐,等.华中地区冬季灰霾天气下PM2.5中重金属污染特征及健康风险评价:以湖北黄冈为例[J].环境科学,2021,42(10):4593-4601.[LI Xing-yu,MAO Yao,CHEN Zhan-le,et al.Characteristics and Health Risk Assessment of Heavy Metals in PM2.5 under Winter Haze Conditions in Central China:A Case Study of Huanggang,Hubei Province[J].Environmental Science,2021,42(10):4593-4601.]
[26]	沈建东,周玉强,王蕴赟,等.杭州西湖景区PM2.5中重金属来源及健康风险评价[J].环境污染与防治,2020,42(2):199-203.[SHEN Jian-dong,ZHOU Yu-qiang,WANG Yun-yun,et al.Sources and Health Risk Assessment of Heavy Metals in PM2.5 of West Lake Scenic Area in Hangzhou[J].Environmental Pollution & Control,2020,42(2):199-203.]
[27]	周梦帆,钱新,李慧明,等.南京仙林地区大气PM2.5中金属化学形态分析及其风险评估[J].环境污染与防治,2020,42(6):767-774.[ZHOU Meng-fan,QIAN Xin,LI Hui-ming,et al.Fractionation of Airborne PM2.5-bound Metals and Associated Risks in Xianlin Area of Nanjing[J].Environmental Pollution & Control,2020,42(6):767-774.]
[28]	耿源濛,张传兵,张勇,等.我国城市污泥中重金属的赋存形态与生态风险评价[J].环境科学,2021,42(10):4834-4843.[GENG Yuan-meng,ZHANG Chuan-bing,ZHANG Yong,et al.Speciation and Ecological Risk Assessment of Heavy Metals in the Municipal Sewage Sludge of China[J].Environmental Science,2021,42(10):4834-4843.]
[29]	FAN M Y,ZHANG Y L,LIN Y C,et al.Specific Sources of Health Risks Induced by Metallic Elements in PM2.5 during the Wintertime in Beijing,China[J].Atmospheric Environment,2021,246:118112.
[30]	WANG X,WANG B,XIAO L L,et al.Sources of 24-h Personal Exposure to PM2.5-bound Metals:Results from a Panel Study in Wuhan,China[J].Environmental Science and Pollution Research,2021,28(22):27555-27564.
[31]	FANG B,ZENG H,ZHANG L,et al.Toxic Metals in Outdoor/Indoor Airborne PM2.5 in Port City of Northern,China:Characteristics,Sources,and Personal Exposure Risk Assessment[J].Environmental Pollution,2021,279:116937.
[32]	闫广轩,张朴真,黄海燕,等.郑州-新乡冬季PM2.5中元素浓度特征及其源分析[J].环境科学,2019,40(5):2027-2035.[YAN Guang-xuan,ZHANG Pu-zhen,HUANG Hai-yan,et al.Concentration Characteristics and Source Analysis of PM2.5 during Winter Time in Zhengzhou-Xinxiang[J].Environmental Science,2019,40(5):2027-2035.]