1. College of Environment and Climate, Institute for Environmental and Climate Research, Jinan University, Guangzhou 511443, China; 2. Guangzhou Regional Low Carbon Economy Research Base, Jinan University, Guangzhou 510632, China; 3. Guangdong Province Foshan Ecology and Environment Monitoring Station, Foshan 528010, China; 4. Guangdong Ecological Environment Monitoring Centre, Guangzhou 510308; 5. Key Laboratory of Regional Air Quality Monitoring for Environmental Protection, Ministry of Ecology and Environment, Guangzhou 510308; 6. Hong Kong University of Science and Technology (Guangzhou), Thrust of Sustainable Energy and Environment, Guangzhou 511458, China
Abstract：In response to issues identified in the polycyclic aromatic hydrocarbons (PAHs) emission inventory for Guangdong Province—including time-lag, unclear source classification, and ambiguous emission trends—a refined PAHs emission factor library for anthropogenic sources was established through comprehensive literature research. A high-resolution, bottom-up PAHs emission inventory of 16PAH compounds for Guangdong Province covering 2006~2020 was developed using the emission factor method, providing insights into principal emission species, key sources, and the spatiotemporal evolution of emissions. The findings were as follows: From 2006 to 2020, anthropogenic PAHs emissions in Guangdong Province showed an overall decline of 45%, with the contribution of carcinogenic PAHs reducing from 60% to 29%. Naphthalene (Nap), benzo[g,h,i]perylene (Bghip), and phenanthrene (Phe) emerged as the primary PAH species, contributing on average 23%, 10%, and 9% to total PAHs emissions, respectively. As national standards for diesel vehicles and motorcycles tightened, yellow-label vehicles were eliminated, and policies like the prohibition on straw burning were enacted, the primary sources of PAHs emissions shifted from motorcycles, diesel vehicles, and biomass burning to industrial coal combustion, coking, and household combustion. Spatial analysis indicated that line-source emissions (primarily from motorcycles and diesel vehicles) decreased significantly, while point-source emissions from industrial sources increased across several regions. Considering population health risks and the need for targeted PAHs emission controls in densely populated areas, the study recommends enhanced regulation of PAHs from industrial coal combustion and coking industries. This study provides critical scientific support for Guangdong Province's PAHs emission control strategies, with a focus on public health outcomes.
[1] Patnaik P. A Comprehensive guide to the properties of hazardous chemical substances [M]. 3th ed. New YorkJ:ohn Wiley and Sons Publishers, 1999. [2] 郭 建,罗孝俊,管克兰,等.石化工业园员工PAHs的皮肤暴露及健康风险 [J]. 中国环境科学, 2022,42(11):5427-5435. Guo J, Luo X J, Guan K L, et al. Skin exposure to PAHs and health risks among employees in a petrochemical industrial park [J]. China Environmental Science, 2022,42(11):5427-5435. [3] 车 凯,郁金星,刘松涛,等.河北南部变电站场地土壤中PAHs含量、来源及健康风险 [J]. 中国环境科学, 2020,40(11):4865-4874. Che K, Yu JX, Liu ST, et al. PAHs content, sources, and health risks in the soil of a substation site in southern Hebei [J]. China Environmental Science, 2020,40(11):4865-4874. [4] Li C, Li Z, Wang H. Characterization and risk assessment of polycyclic aromatic hydrocarbons (PAHs) pollution in particulate matter in rural residential environments in China-A review [J]. Sustainable Cities and Society, 2023,96,104690-104704. [5] 冯承莲,雷炳莉,王子健.中国主要河流中多环芳烃生态风险的初步评价 [J]. 中国环境科学, 2009,29(6):583-588. Feng C L, Lei B L, Wang Z J. Preliminary assessment of ecological risks of polycyclic aromatic hydrocarbons in major rivers of China [J]. China Environmental Science, 2009,29(6):583-588. [6] Dat N D, Chang M B. Review on characteristics of PAHs in atmosphere, anthropogenic sources and control technologies [J]. Science of the Total Environment, 2017,609:682-693. [7] Humel S, Schmidt S N, Sumetzberger-Hasinger M, et al. Enhanced accessibility of polycyclic aromatic hydrocarbons (PAHs) and heterocyclic PAHs in industrially contaminated soil after passive dosing of a competitive sorbate [J]. Environmental Science & Technology, 2017,51(14):8017-8026. [8] Du W, Yun X, Chen Y, et al. PAHs emissions from residential biomass burning in real-world cooking stoves in rural China [J]. Environmental Pollution, 2020,267:115592-115599. [9] Sun J, Shen Z, Zeng Y, et al. Characterization and cytotoxicity of PAHs in PM2.5emitted from residential solid fuel burning in the Guanzhong Plain, China [J]. Environmental Pollution, 2018,241:359-368. [10] Manoli E, Samara C. Polycyclic aromatic hydrocarbons in natural waters: sources, occurrence and analysis [J]. TrAC Trends in Analytical Chemistry, 1999,18(6):417-428. [11] Gong P, Wang X. Forest fires enhance the emission and transport of persistent organic pollutants and polycyclic aromatic hydrocarbons from the central himalaya to the tibetan plateau [J]. Environmental Science & Technology Letters, 2021,8(7):498-503. [12] Mallah M A, Changxing L, Mallah M A, et al. Polycyclic aromatic hydrocarbon and its effects on human health: An overeview [J]. Chemosphere, 2022,296:133948-133963. [13] Du W, Chen Y, Zhu X, et al. Wintertime air pollution and health risk assessment of inhalation exposure to polycyclic aromatic hydrocarbons in rural China [J]. Atmospheric Environment, 2018,191:1-8. [14] Chen L Y, Liu W J, Tao S, et al. Spatiotemporal variations and source identification of atmospheric nitrated and oxygenated polycyclic aromatic hydrocarbons in the coastal cities of the Bohai and Yellow Seas in northern China [J]. Chemosphere, 2021,279:130565-130577. [15] Mu L, Li X, Liu X, et al. Characterization and emission factors of carbonaceous aerosols originating from coke production in China [J]. Environmental Pollution, 2021,268:115768-115775. [16] Shen H, Huang Y, Wang R, et al. Global atmospheric emissions of polycyclic aromatic hydrocarbons from 1960to 2008and future predictions [J]. Environmental Science & Technology, 2013,47(12):6415-6424. [17] Zhang Y, Tao S. Global atmospheric emission inventory of polycyclic aromatic hydrocarbons (PAHs) for 2004 [J]. Atmospheric Environment, 2009,43(4):812-819. [18] 中华人民共和国环境保护部,工业和信息化部,国家卫生和计划生育委员会.关于发布《优先控制化学品名录(第一批)》的公告[EB/OL]. [公告 2017年 第83号]. 20171227.https://www.mee.gov.cn/gkml/hbb/bgg/201712/t20171229_428832.htm?tdsourcetag=s_pcqq_aiomsg. Ministry of Environmental Protection of the People's Republic of China, Ministry of Industry and Information Technology, National Health and Family Planning Commission. Announcement on the release of the "Priority control chemicals list (first batch)" [EB/OL]. [Announcement No. 83 of 2017]. 20171227. [19] 中华人民共和国生态环境部,工业和信息化部,国家卫生健康委员会. 关于发布《优先控制化学品名录(第二批)》的公告［EB/OL］. [公告 2020年 第47号]. 20201030.https://www.mee.gov.cn/xxgk2018/xxgk/xxgk01/202011/t20201102_805937.html. Ministry of Ecology and Environment of the People's Republic of China, Ministry of Industry and Information Technology, National Health Commission. Announcement on the release of the "Second batch of priority control chemicals list" [EB/OL]. [Announcement No. 47 of 2020]. [20] 徐 徐.中国大气中人为多环芳烃排放对人群健康影响的研究 [D]. 济南:山东大学, 2014. Xu X. Polycyclic aromatic hydrocarbons air pollution generated from human activity and its human health impact in China [D]. Jinan, Shandong University, 2014. [21] Zhang P, Zhou Y, Chen Y, et al. Construction of an atmospheric PAH emission inventory and health risk assessment in Jiangsu, China [J]. Air Quality, Atmosphere & Health, 2023,16(3):629-640. [22] Cui H, Lu Y, Zhou Y, et al. Spatial variation and driving mechanism of polycyclic aromatic hydrocarbons (PAHs) emissions from vehicles in China [J]. Journal of Cleaner Production, 2022,336:130210-130222. [23] Zhao T, Yang L, Huang Q, et al. PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) and nitrated-PAHs (NPAHs) emitted by gasoline vehicles: Characterization and health risk assessment [J]. Science of the Total Environment, 2020,727:138631-138640. [24] 郑 轩.基于车载测试的重型柴油车黑碳与多环芳烃排放特征研究 [D]. 北京:清华大学, 2016. Zheng X, Emission characteristicsof black carbon and polycyclic aromatic hydrocarbonfrom heavy duty diesel vehiclesBased on PEMS Method [D]. Beijing, Tsinghua University, 2016. [25] Li B, Zhou S, Wang T, et al. An improved gridded polycyclic aromatic hydrocarbon emission inventory for the lower reaches of the Yangtze River Delta region from 2001 to 2015 using satellite data [J]. Journal of Hazardous Materials, 2018,360:329-339. [26] 蒋秋静,李跃宇,胡新新,等.太原市多环芳烃(PAHs)排放清单与分布特征分析 [J]. 中国环境科学, 2013,33(1):14-20. Jiang QJ, Li YY, Hu XX, et al. Emission inventory and distribution characteristics analysis of polycyclic aromatic hydrocarbons (PAHs) in Taiyuan City [J]. China Environmental Science, 2013,33(1):14-20. [27] 王翠萍.广东省主要持久性有机污染物排放状况的初步研究 [D]. 广州:中国科学院研究生院(广州地球化学研究所), 2007. Wang C P. Preliminary study on the emission situation of the main persistant organic pollutants in Guangdong Province, China [D]. Guangzhou, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, 2007. [28] 国家统计局能源统计司.中国能源统计年鉴(2006~2020) [M]. 北京:中国统计出版社, 2021. Energy Statistics Department of the National Bureau of Statistics. China energy statistical yearbook (2006~2020) [M]. Beijing: China Statistics Press, 2021. [29] 广东省统计局.广东统计年鉴(2006~2020) [M]. 北京:中国统计出版社, 2021. Guangdong Provincial Bureau of Statistics. Guangdong statistical yearbook (2006~2020) [M]. Beijing: China Statistics Press, 2021. [30] 郑君瑜,王水胜,黄志炯,等.区域高分辨率大气排放源清单建立的技术方法与应用 [M]. 北京:科学出版社, 2014. Zheng J Y, Wang S S, Huang Z J, et al. Technical methods and applications for establishing regional high-resolution atmospheric emission inventories [M]. Beijing: Science Press, 2014. [31] 中国港口年鉴编辑部.中国港口年鉴(2006~2020) [M]. 北京:中国港口杂志社, 2021. Editorial Office of China Ports Yearbook. China ports yearbook (2006~2020) [M]. Beijing: China Ports Magazine Press, 2021. [32] 广东农村统计年鉴编辑委员会.广东省农村统计年鉴(2006~2020) [M]. 北京:中国统计出版社, 2021. Editorial Committee of Guangdong Rural Statistical Yearbook. Guangdong rural statistical yearbook (2006~2020) [M]. Beijing: China Statistics Press, 2021. [33] 中国交通年鉴编辑部.中国交通年鉴(2006~2020) [M]. 北京:中国交通出版社, 2021. Editorial Office of China Communications Yearbook. China communications yearbook (2006~2020) [M]. Beijing: China Communications Press, 2021. [34] 王伯光,吕万明,周 炎,等.城市隧道汽车尾气中多环芳烃排放特征的研究 [J]. 中国环境科学, 2007,(4):482-487. Tian B G, LV W M, Zhou Y, et al. Emission characteristic of PAHs composition in motor vehicles exhaust of city tunnel [J]. China Environmental Science, 2007,(4):482-487. [35] Adam T, Farfaletti A, Montero L, et al. Chemical characterization of emissions from modern two-stroke mopeds complying with legislative regulation in Europe (EURO-2) [J]. Environmental Science & Technology, 2010,44(1):505-512. [36] Spezzano P, Picini P, Cataldi D, et al. Particle-phase polycyclic aromatic hydrocarbon emissions from non-catalysed, in-use four- stroke scooters [J]. Environmental monitoring and assessment, 2007, 133:105-117. [37] Spezzano P, Picini P, Cataldi D, et al. Particle-and gas-phase emissions of polycyclic aromatic hydrocarbons from two-stroke, 50cm3 mopeds [J]. Atmospheric Environment, 2008,42(18):4332-4344. [38] Yang H H, Hsieh L T, Liu H C, et al. Polycyclic aromatic hydrocarbon emissions from motorcycles [J]. Atmospheric Environment, 2005,39 (1):17-25. [39] Chen F, Hu W, Zhong Q. Emissions of particle-phase polycyclic aromatic hydrocarbons (PAHs) in the Fu Gui-shan Tunnel of Nanjing, China [J]. Atmospheric Research, 2013,124:53-60. [40] Alves C A, Barbosa C, Rocha S, et al. Elements and polycyclic aromatic hydrocarbons in exhaust particles emitted by light-duty vehicles [J]. Environmental Science and Pollution Research, 2015, 22:11526-11542. [41] Fang X, Wu L, Zhang Q, et al. Characteristics, emissions and source identifications of particle polycyclic aromatic hydrocarbons from traffic emissions using tunnel measurement [J]. Transportation Research Part D: Transport and Environment, 2019,67:674-684. [42] Hao X, Zhang X, Cao X, et al. Characterization and carcinogenic risk assessment of polycyclic aromatic and nitro-polycyclic aromatic hydrocarbons in exhaust emission from gasoline passenger cars using on-road measurements in Beijing, China [J]. Science of the Total Environment, 2018,645:347-355. [43] Ho K F, Ho S S H, Lee S C, et al. Emissions of gas-and particle-phase polycyclic aromatic hydrocarbons (PAHs) in the Shing Mun Tunnel, Hong Kong [J]. Atmospheric Environment, 2009,43(40):6343-6351. [44] Kristensson A, Johansson C, Westerholm R, et al. Real-world traffic emission factors of gases and particles measured in a road tunnel in Stockholm, Sweden [J]. Atmospheric Environment, 2004,38(5):657-673. [45] Liu Y, Wang S, Lohmann R, et al. Source apportionment of gaseous and particulate PAHs from traffic emission using tunnel measurements in Shanghai, China [J]. Atmospheric Environment, 2015,107:129-136. [46] Liu Y, Gao Y, Yu N, et al. Particulate matter, gaseous and particulate polycyclic aromatic hydrocarbons (PAHs) in an urban traffic tunnel of China: Emission from on-road vehicles and gas-particle partitioning [J]. Chemosphere, 2015,134:52-59. [47] Louis C, Liu Y, Tassel P, et al. PAH, BTEX, carbonyl compound, black-carbon, NO2and ultrafine particle dynamometer bench emissions for Euro 4 and Euro 5diesel and gasoline passenger cars [J]. Atmospheric Environment, 2016,141:80-95. [48] Wang X, Khlystov A, Ho K F, et al. Real-world vehicle emissions characterization for the shing mun tunnel in Hong Kong and Fort McHenry Tunnel in the United States [J]. Research Reports: Health Effects Institute, 2019,199:5-52. [49] Zhang Y, Wang X, Li G, et al. Emission factors of fine particles, carbonaceous aerosols and traces gases from road vehicles: recent tests in an urban tunnel in the Pearl River Delta, China [J]. Atmospheric Environment, 2015,122:876-884. [50] Zheng X, Zhang S, Wu Y, et al. Measurement of particulate polycyclic aromatic hydrocarbon emissions from gasoline light-duty passenger vehicles [J]. Journal of Cleaner Production, 2018,185:797-804. [51] Xu S, Liu W, Tao S. Emission of polycyclic aromatic hydrocarbons in China [J]. Environmental Science & Technology, 2006,40(3):702-708. [52] 李保杰.南京大气多环芳烃的时空分布特征与模拟 [D]. 南京:南京大学, 2016. Li B J. The Spatio-temporal Distribution of Atmospheric Gaseous PAHs Concentration and Numerical Simulation in Nanjing [D]. Nanjing, Najing University, 2016. [53] Wang L, Du W, Yun X, et al. On-site measured emission factors of polycyclic aromatic hydrocarbons for different types of marine vessels [J]. Environmental Pollution, 2022,297:118782-118790. [54] Wang J, Du W, Chen Y, et al. Nitrated and oxygenated polycyclic aromatic hydrocarbons emissions from solid fuel combustion in rural China: Database of 12real-world scenarios for residential cooking and heating activities [J]. Science of the Total Environment, 2022,852: 158501-158507. [55] 邹昃灏,赵时真,田乐乐,等.珠江三角洲城市大气中多环芳烃的污染特征、来源解析和健康风险评估 [J]. 地球化学, 2021,50(6):644-653. Zou Z H, Zhao S Z, Tian L L, et al. Pollution characteristics, source apportionment, and health risk assessment of polycyclic aromatic hydrocarbons in urban atmosphere of the Pearl River Delta [J]. Geochemistry, 2021,50(6):644-653. [56] Mu L, Peng L, Cao J, et al. Emissions of polycyclic aromatic hydrocarbons from coking industries in China [J]. Particuology, 2013, 11(1):86-93. [57] Nisbet I C T, Lagoy P K. Toxic equivalency factors (TEFs) for polycyclic aromatic hydrocarbons (PAHs) [J]. Regulatory Toxicology and Pharmacology, 1992,16(3):290-300. [58] Dat N D, Chang M B. Review on characteristics of PAHs in atmosphere, anthropogenic sources and control technologies [J]. Science of the Total Environment, 2017,609:682-693. [59] 明桂英,朱曼妮,沙青娥,等.2006~2020年广东省大气甲醛排放演变特征 [J]. 环境科学, 2023,44(9):4819-4831. Ming G Y, Zhu M N, Sha Q E, et al. Evolution characteristics of atmospheric formaldehyde emissions in Guangdong Province from 2006 to 2020 [J]. Environmental Science, 2023,44(9):4819-4831. [60] 牛计伟,李晓恒,季佳佳,等.2016~2022年珠三角地区PM2.5中多环芳烃污染特征及健康风险 [J]. 环境卫生学杂志, 2024,14(5):431-437. Niu J W, Li X H, Ji J J, et al. Pollution characteristics and health risks of polycyclic aromatic hydrocarbons in PM2.5 in the Pearl River Delta region from 2016 to 2022 [J]. Journal of Environmental Health, 2024, 14(5):431-437.
