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Source apportionment and health risk assessment of metal elements in PM1 on different weather types during autumn and winter-A case study of Qingdao |
DU Jin-hua1, TAO Wen-xin1, ZHANG Yi-sheng1, LIU Zi-yang2, YANG Jian-li1, ZHANG Su-fan1, WANG Chao-long1, CUI Shan-shan1, XUE-Lian3, ZHANG Hou-yong4, SUN Ying-jie1 |
1. School of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266520, China; 2. Institute for Environmental and Climate Research, Jinan University, Guangzhou 511400, China; 3. Qingdao Eco-environment Monitoring Center of Shandong Province, Qingdao 266003, China; 4. Ji'nan Eco-environment Monitoring Center of Shandong Province, Jinan 250102, China |
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Abstract Over four consecutive autumn-winter seasons spanning from 2018 to 2022, a comprehensive analysis was conducted involving daily sampling of atmospheric PM1 and the subsequent examination of 20 distinct metal elements. The characteristics and sources of metal elements under different weather conditions were analyzed, and their health risks were assessed. The results revealed that on dust days, metal element content (2022.88±2298.00) ng/m3 and their proportion in PM1 (6.63%) were higher compared to other weather conditions. Specifically, the metal element content on haze and polluted fog days was 2.06 and 1.70 times higher than on clean days. Carcinogenic metal elements (Ni, Cd, As, Cr, Co, and Pb) and non-carcinogenic metal elements (Mn, Zn, Cu, V, Al, and Ba) showed higher enrichment factors on haze and polluted fog days. Positive matrix factorization (PMF) analysis identified primary sources of metal elements in PM1, including vehicular emissions, coal/biomass combustion, sea salt, crustal sources, industrial emissions, and maritime sources. Vehicular emissions and coal/biomass combustion notably contributed over 72.1% during foggy and hazy days, while maritime sources increased to 1.9% on clear fog days. Backward air trajectory analysis demonstrated that haze days were mainly affected by the transmission of pollutants from northwest to medium and long distances. Ocean-land circulation mainly affected polluted fog days, while dust days were dominated by long-distance transport of northwest dust masses. The non-carcinogenic risks via respiratory exposure to metallic elements in PM1 were deemed negligible. However, the lifetime carcinogenic risks of As and Cr exceeded the threshold of 10-6 but remained below 10-4, with the highest risk probability observed during polluted fog and haze days. Consequently, it's recommended to intensify emission control measures targeting As and Cr sources in industrial processes such as coal combustion, metallurgy, and electroplating, particularly during heavy pollution episodes in autumn and winter.
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Received: 04 January 2024
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Corresponding Authors:
张宜升,副教授,doctorzys@163.com
E-mail: doctorzys@163.com
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[1] Schneider I L, Teixeira E C, Agudelo-Castaneda D M, et al. FTIR analysis and evaluation of carcinogenic and mutagenic risks of nitro-polycyclic aromatic ydrocarbons in PM1.0 [J]. Science of the Total Environment, 2016,541:1151-1160. [2] Chen J L, Tian N Y, Xu H. Solid-phase microextraction of volatile organic compoundsin headspace of PM-induced MRC-5cell lines[J]. Talanta, 2018,185:23-29. [3] Galindo N, Yubero E, Nicolas J F, et al. Characterization of metals in PM1 and PM10 and health risk evaluation at an urban site in the western Mediterranean [J]. Chemosphere, 2018,201:243-250. [4] Chen G, Morawska L, Zhang W, et al. Spatiotemporal variation of PM1 pollution in China [J]. Atmospheric Environment, 2018,178:198-205. [5] Yang B Y, Guo Y, Bloom M S, et al. Ambient PM1air pollution, blood pressure, and hypertension: Insights from the 33Communities Chinese Health Study [J]. Environmental Research, 2019,170:252-259. [6] Vecchi R, Marcazzan G, Valli G, et al. The role of atmospheric dispersion in the seasonal variation of PM1 and PM2.5 concentration and composition in the urban area of Milan (Italy) [J]. Atmospheric Environment, 2004,38(27):4437-4446. [7] Zhang Y Y, Lang J L, Cheng S Y, et al. Chemical composition and sources of PM1 and PM2.5 in Beijing in autumn [J]. Science of the Total Environment, 2018,630:72-82. [8] Agudelo-Castaneda D M, Teixeira E C, Schneider I L, et al. Exposure to polycyclic aromatic hydrocarbons in atmospheric PM1.0 of urban environments: Carcinogenic and mutagenic respiratory health risk by age groups [J]. Environmental Pollution, 2017,224:158-170. [9] Li R, Guo J P, Geng G N, et al. Satellite-derived long-term estimates of full-coverage PM1 concentrations across China based on a stacking decision tree model [J]. Atmospheric Environment, 2021,255,doi:10. 1016/j.atmosenv.2021.118448. [10] GBD 2019Risk Factors Collaborators. Global burden of 87 risk factors in 204 countries and territories, 1990~2019: a systematic analysis for the Global Burden of Disease Study 2019[J]. Lancet, 2020,396(10258):1223-1249. [11] Hu K, Guo Y, Hu D, et al. Mortality burden attributable to PM1 in Zhejiang province, China [J]. Environment International, 2018,121(Pt 1):515-522. [12] 江琪,王飞,孙业乐.河北香河亚微米气溶胶组分特性、来源及其演变规律分析[J]. 环境科学, 2018,39(3):3022-3032. Jiang Q, Wang F, Sun Y L. Analysis of chemical composition, source and evolution of submicron particles in Xianghe, Hebei province [J]. Environmental Science, 2018,39(3):3022-3032. [13] 邢琼予,戴启立,毕晓辉,等.我国中西部典型城市PM2.5中痕量金属的时空分布特征和健康影响[J]. 中国环境科学, 2019,39(2):574- 582. Xing Q Y, Dai Q L, Bi X H, et al. Temporal-spatial variation and health effects of trace metals in PM2.5 in four central-western cities of China [J]. China Environmental Sciences, 2019,39(2):574-582. [14] Prakash J, Lohia T, Mandariya A K, et al.Chemical characterization and quantitative assessment of source-specific health risk of trace metals in PM1.0 at a road site of Delhi, India [J]. Environmental Science and Pollution Research, 2018,25(9):8747-8764. [15] Wang K, Wang W Y, Li L L, et al. Seasonal concentration distribution of PM1.0 and PM2.5 and a risk assessment of bound trace metals in Harbin, China: Effect of the species distribution of heavy metals and heat supply [J]. Scientific Reports, 2020,10(1),doi:10.1038/s 41598- 020-65187-7. [16] Yang B Y, Guo Y, Morawska L, et al. Ambient PM1 air pollution and cardiovascular disease prevalence: insights from the 33 Communities Chinese Health Study [J]. Environment International, 2018,123: 310-317. [17] 石晓兰,宗政,彭辉,等.近10年华北背景大气PM2.5中重金属健康风险及污染来源的变化[J]. 环境科学, 2023,44(10):5335-5343. Shi X L, Zong Z, Peng H, et al. Changes in health risks and pollution sources of atmospheric PM2.5-bound metals in a background site in North China [J]. Environmental Science, 2023,44(10):5335-5343. [18] Guo J H, Zhou J Y, Han R Q, et al. Association of short-term co-exposure to particulate matter and Ozone with mortality risk [J]. Environmental Science & Technology, 2023,57:15825-15834. [19] 王进进.四川典型城市大气PM1的理化特征、同位素源解析及健康风险评价[D]. 成都:成都理工大学, 2021. Wang J J. Physical and chemical characteristics, isotope source tracer and health risk assessment of PM1 in typical cities of Sichuan Province [D]. Chengdu: Chengdu University of Technology, 2021. [20] 刘子杨,张宜升,张厚勇,等.青岛秋冬季PM1中金属元素污染特征及健康风险评估[J]. 环境科学, 2022,43(9):4448-4457. Liu Z Y, Zhang Y S, Zhang H Y, et al. Characteristics and health risk assessment of trace elements in atmospheric PM1 during autumn and winter in Qingdao [J]. Environmental Science, 2022,43(9):4448-4457. [21] Galindo N, Yubero E, Nicolas J F, et al. Characterization of metals in PM1 and PM10 and health risk evaluation at an urban site in the western [J]. Mediterranean. Chemosphere, 2018,201:243-250. [22] Gao J, Wei Y T, Shi G L, et al. Roles of RH, aerosol pH and sources in concentrations of secondary inorganic aerosols, during different pollution periods [J]. Atmospheric Environment, 2020,241:117770. [23] Wang H J, Chen H P. Understanding the Recent Trend of Haze Pollution in Eastern China: Roles of Climate Change [J]. Atmospheric Chemistry and Physics, 2016,16(6):4205-4211. [24] 彭倩倩,刘晓环,杜金花,等.青岛冬季霾-沙尘重污染过程PM1理化特征及来源分析[J]. 中国环境科学, 2020,40(9):3731-3740. Peng Q Q, Liu X H, Du J H, et al. Physicochemical characteristics and source analysis of PM1 during winter haze-dust pollution event in Qingdao [J]. China Environmental Science, 2020,40(9):3731-3740. [25] 卢一凡,王娇,于铖浩,等.青岛市雾、霾天时空变化特征及影响因素分析[J]. 中国海洋大学学报(自然科学版), 2021,51(7):34-45. Lu Y F, Wang J, Yu C H, et al. Temporal-spatial variation characteristics and influence factors of fog and haze events in Qingdao, China [J]. Periodical of Ocean University of China, 2021,51(7):34-45. [26] 庹雄,杨凌霄,张婉,等.海-陆大气交汇作用下青岛冬季PM2.5污染特征与来源解析[J]. 环境科学, 2020,43(5):2284-2293. Tuo X, Yang L X, Zhang W, et al. Characteristics and source analysis of PM2.5 in Qingdao in winter under the action of sea-land- atmosphere convergence [J]. Environmental Science, 2020,43(5): 2284-2293. [27] Chen D S, Wang X T, Nelson P, et al. Ship emission inventory and its impact on the PM2.5 air pollution in Qingdao Port, North China [J]. Atmospheric Environment, 2017,166:351-361. [28] 姚青,韩素芹,蔡子颖.天津采暖期大气PM2.5中重金属元素污染及其生态风险评价[J]. 中国环境科学, 2013,33(9):1596-1600. Yao Q, Han S Q, Cai Z Y. The pollution characteristics and potential ecological risk of heavy metals in PM2.5 during heating season in Tianjin [J]. China Environmental Sciences, 2013,33(9):1596-1600. [29] 王申博,王玲玲,范相阁,等.河南省北部区域霾污染过程中城市和农村点位PM2.5组分差异[J]. 环境科学, 2023,44(1):11-19. Wang S B, Wang L L, Fan X G, et al. Differences in PM2.5 components between urban and rural sites during heavy haze event in northern Henan province [J]. Environmental Science, 2023,44(1):11-19. [30] 张思蕊,樊曙先,王元,等.南京雾过程对大气气溶胶谱分布及化学组成的影响[J]. 中国环境科学, 2022,42(11):4961-4973. Zhang S R, Fan S X, Wang Y, et al. Effects of Nanjing fog process on the spectral distribution and chemical composition of atmospheric aerosols [J]. China Environmental Science, 2022,42(11):4961-4973. [31] 管阳,石金辉.雾霾天对青岛PM2.5中铁、磷浓度及溶解度的影响[J]. 中国海洋大学学报(自然科学版), 2021,51(4):117-125. Guan Y, Shi J H. Concentration and solubility of iron and phosphorus in PM2.5 in hazy and foggy air at the coastal city Qingdao of China [J]. Periodical of Ocean University of China, 2021,51(4):117-125. [32] 王耀庭,李青春,郑祚芳,等.北京春季一次霾-沙天气污染特性与成因分析[J]. 环境科学, 2019,40(6):2582-2594. Wang Y T, Li Q C, Zheng Z F, et al. Research on the pollution characteristics and causality of haze-sand air pollution in Beijing in spring [J]. Environmental Science, 2019,40(6):2582-2594. [33] 邓林俐,张凯山,殷子渊,等.基于PMF模型的PM2.5中金属元素污染及来源的区域特征分析[J]. 环境科学, 2020,41(12):5276-5287. Deng L L, Zhang K S, Yin Z Y, et al. Characterization of metal pollution of regional atmospheric PM2.5 and its sources based on the PMF model [J]. Environmental Science, 2020,41(12):5276-5287. [34] Xu B, Xu H, Zhao H, et al. Source apportionment of fine particulate matter at a megacity in China, using an improved regularization supervised PMF model [J]. Science of The Total Environment, 2023,879:163198. [35] 张天力,黄小娟,张军科,等.川南城市群冬季大气细颗粒物中金属元素特征及其来源解析[J/OL]. 环境科学, https://doi.org/10.13227/ j.hjkx.202305089. Zhang T L, Huang X J, Zhang J K, et al. Characterization of metal elements in atmospheric fine particulate matter and their sources in winter in the southern Sichuan urban agglomeration [J/OL]. Environmental Science, https://doi.org/10.13227/j.hjkx.202305089. [36] 陶文鑫,谭玉冉,张宜升,等.海运低硫管控政策下青岛PM2.5和PM1金属元素污染特征及来源解析[J]. 中国环境科学, 2023,43(7): 3339-3349. Tao W X, Tan Y R, Zhang Y S, et al. Characteristics and source analysis of PM2.5 and PM1 metal elements in Qingdao under marine low-sulfur regulation [J]. China Environmental Science, 2023,43(7): 3339-3349. [37] Wang Y, Zhang X, Draxler R R. TrajStat: GIS-based software that uses various trajectory statistical analysis methods to identify potential sources from long-term air pollution measurement data [J]. Environmental Modeling & Software, 2009,24(8):938-939. [38] 古添发,闫润华,姚沛廷,等.深圳市大气中PM2.5载带金属污染特征及健康风险[J]. 中国环境科学, 2023,43(1):88-95. Gu T F, Yan R H, Yao P T, et al. Characteristics and health risks of ambient PM2.5-bound metals in Shenzhen [J]. China Environmental Science, 2023,43(1):88-95. [39] Wang S S, Hu G G, 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. [40] 环境保护部.中国人群暴露参数手册(成人卷) [M].北京:中国环境出版社, 2013. Ministry of Environmental Protection. Handbook of Exposure Parameters for the Chinese Population (Adult Volume) [M]. Beijing: China Environmental Publishing House, 2013. [41] 吴凯章,刘明,罗中华,等.大宝山多金属矿区周边大气重金属来源解析与风险评估[J/OL]. 中国环境科学, https://doi.org/10.19674/ j.cnki.issn1000-6923.20230811.001. Wu K Z, Liu M, Luo Z H, et al. Sources apportionment and risk assessment of atmospheric heavy metals in the vicinity of Dabao Mountain polymetallic mining area [J]. China Environmental Science, https://doi.org/10.19674/j.cnki.issn1000-6923.20230811.001. [42] Huang R J, Cheng R, Jing M, et al. Source-specific health risk analysis on particulate trace elements: coal combustion and traffic emission as major contributors in wintertime Beijing [J]. Environmental Science & Technology, 2018,52(19):10967-10974. [43] Zhu W H, Xu X D, Zheng J, et al. The characteristics of abnormal wintertime pollution events in the Jing-Jin-Ji Region and its relationships with meteorological factors [J]. Science of the Total Environment, 2018,626:887-898. [44] Han S Q, Wu J H, Zhang YF, et al. Characteristics and formation mechanism of a winter haze-fog episode in Tianjin, China [J]. Atmospheric Environment, 2014,98:323-330. [45] Li, J, Gao W, Cao L, et al. Significant changes in autumn and winter aerosol composition and sources in Beijing from 2012 to 2018: effects of clean air actions [J]. Environmental Pollution, 2021,268:115855.1- 10. [46] Huang X F, Li X, He L Y, et al. 5-year study of rainwater chemistry in a coastal mega-city in South China [J]. Atmospheric Research, 2010, 97(1/2):185-193. [47] 李瑞芃,石金辉,张代洲,等.天气条件及气团来源对青岛春季大气颗粒物数浓度谱分布的影响[J]. 中国环境科学, 2012,32(8):1392- 1399. Li R F, Shi J H, Zhang D Z, et al. Size distribution of atmospheric particles in number concentration in relation to meteorological conditions and air mass origins in Qingdao in spring [J]. China Environmental Science, 2012,32(8):1392-1399. [48] 沈利娟,施双双,郭振东,等.长三角沙尘中气溶胶粒径分布及化学组分特征[J]. 中国环境科学, 2019,39(6):2241-2248. Shen L J, Shi S S, Guo Z D, et al. Characteristics of aerosol size distribution and chemical components during a dust pollution episode in the Yangtze River Delta [J]. China Environmental Science, 2019, 39(6):2241-2248. [49] Zhang H R, Li S, Dong F, et al. Abundance and fractional solubility of aerosol iron during winter at a coastal city in Northern China: similarities and contrasts between fine and coarse particles [J]. Journal of geophysical research: atmospheres, 127,e2021JD036070,10.1029/ 2021JD036070. [50] Wang K, Wang W Y, Li L L, et al. Seasonal concentration distribution of PM1.0 and PM2.5 and a risk assessment of bound trace metals in Harbin, China: Effect of the species distribution of heavy metals and heat supply [J]. Scientific Reports, 2020,10(1),doi:10.1038/s41598- 020-65187-7. [51] Cheng Y, Zou S C, Lee S C, et al. Characteristics and source apportionment of PM1 emissions at a roadside station [J]. Journal of Hazardous Materials. 2011:195:82-91. [52] Zhang Y Y, Lang J L, Cheng S Y, et al. Chemical composition and sources of PM1 and PM2.5 in Beijing in autumn [J]. Science of the Total Environment, 2018,630:72-82. [53] 周睿智,闫才青,崔敏,等.山东省大气细颗粒物来源解析的研究现状与展望[J]. 中国环境科学, 2021,41(7):3029-3042. Zhou R Z, Yan C Q, Cui M, et al. Research status and prospects on source apportionment of atmospheric fine particulate matter in Shandong Province [J]. China Environmental Science, 2021,41(7): 3029-3042. [54] Wan D, Yang H, Jin Z, et al. Spatiotemporal trends of atmospheric Pb over the last century across inland China [J]. Science of The Total Environment, 2020,729:138399. [55] Liu T, Hu B, Yang Y, et al. Characteristics and source apportionment of PM2.5 on an island of Southeast China:impact of sea-salt and monsoon [J]. Atmospheric Research, 2020,235:104786. [56] Shang J, Khuzestani R B, Tian J, et al. Chemical characterization and source apportionment of PM2.5 personal exposure of two cohorts living in urban and suburban Beijing [J]. Environmental Pollution, 2019, 246:225-236. [57] Corbin J C, Mensah A A, Pieber S M, et al. Trace metals in soot and PM2.5 from heavy-fuel-oil Combustion in a Marine Engine [J]. Environmental Science & Technology, 2018,52(11):6714-6722. [58] Celo V, Dabek E, Mccurdy M. Chemical characterization of exhaust emissions from selected Canadian marine vessels: The case of trace metals and lanthanoids [J]. Environmental Science & Technology, 2015,49(8):5220-5226. [59] 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 S, Wang Q H, Xue Y 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. [60] Feng J, Yu H, Su X, et al. Chemical composition and source apportionment of PM2.5 during Chinese Spring Festival at Xinxiang, a heavily polluted city in North China: Fireworks and health risks [J]. Atmospheric Research, 2016,182:176-188. [61] Liu Z Y, Zhang H Y, Zhang Y S, et al. Characterization and sources of trace elements in PM1 during autumn and winter in Qingdao, Northern China [J]. Science of The Total Environment, 2022,811:151319. [62] 邢建伟,宋金明,袁华茂,等.青岛近岸区域典型海陆人为交互作用下酸雨的化学特征[J]. 环境化学, 2017,36(2):296-308. Xing J W, Song J M, Yuan H M, et al. Chemical characteristics of acid rain under the representative interaction among sea, land and anthropogenic activities in the coastal area of Qingdao [J]. Environmental Chemistry, 2017,36(2):296-308. [63] 许雅姿,杨亦成,刘永吉,等.典型大气环流对天津市大气PM2.5与O3复合污染的影响特征[J]. 中国环境科学, 2023,43(10):5078-5087. Xu Y Z, Yang Y C, Liu Y J, et al. Impact characteristics of typical atmospheric circulation on the combined pollution of PM2.5 and O3 in Tianjin [J]. China Environmental Science, 2023,43(10):5078-5087. [64] 张吉,黄柳斌,赵敏,等.海陆交换对崂山臭氧和二次气溶胶的影响[J]. 中国环境科学, 2023,43(6):2683-2693. Zhang J, Huang L B, Zhao M, et al. Effects of sea-land exchange on ozone and secondary aerosols in Mount Lao [J]. China Environmental Science, 2023,43(6):2683-2693. [65] 李立伟,邓小文,肖致美,等.天津市采暖季不同气团来向PM2.5中重金属污染特征及健康风险评价[J]. 环境科学, 2023,44(1):30-37. Li L W, Deng X W, Xiao Z M, et al. Pollution characteristics and health risk assessment of heavy metals in PM2.5 of different air masses during heating season in Tianjin [J]. Environmental Science, 2023,44(1):30-37. [66] 李宏艳,赵志新,何秋生,等.山西介休焦化区PM2.5重金属污染特征、关键毒性组分与来源[J]. 中国环境科学, 2023,43(4):1528-1538. Li H Y, Zhao Z X, He Q S, et al. Pollution characteristics, key toxic components and sources of PM2.5-bound heavy metals in coking polluted area of Jiexiu, Shanxi [J]. China Environmental Science, 2023,43(4):1528-1538. [67] 齐霁.短期大气重污染健康损害评估研究[D]. 北京:清华大学, 2020. Qi J. Study on health damage assessment of short-term heavy air pollution [D]. Tsinghua University, 2020. [68] 王显钦,费学海,杨员,等.贵阳市花溪城区PM2.5中重金属元素的污染特征、来源及健康风险评价[J]. 环境科学学报, 2023,43(6): 110-118. Wang X Q, Fei X M, Yang Y, et al. Pollution characteristics, source apportionment and health risk assessment of heavy metal elements in PM2.5 collected in Huaxi urban areas, Guiyang [J]. Acta Scientiae Circumstantiae, 2023,43(6):110-118. [69] 王永越,张芷宁,罗震宇,等.环境空气质量基准和标准制定方法及其对我国的启示[J]. 科学通报, 2022,67(27):3324-3339. Wang Y Y, Zhang Z N, Luo Z Y, et al. Ambient air quality baseline and standard formulation methods and their enlightenment for China. China Science Bulletin, 2022,67:3324-3339. |
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