加入SOA示踪的深圳大气PM2.5受体模型源解析

苏翠平; 孙逸飞; 曹礼明; 王川; 黄晓锋; 何凌燕

PDF(642 KB)

中国环境科学 ›› 2020, Vol. 40 ›› Issue (12) : 5124-5132.

大气污染与控制

加入SOA示踪的深圳大气PM_2.5受体模型源解析

苏翠平¹, 孙逸飞¹, 曹礼明², 王川², 黄晓锋¹, 何凌燕¹

作者信息 +

Source apportionment of PM_2.5 in Shenzhen based on receptor model with SOA tracer

SU Cui-ping¹, SUN Yi-fei¹, CAO Li-ming², WANG Chuan², HUANG Xiao-feng¹, HE Ling-yan¹

Author information +

文章历史 +

摘要

为厘清包括二次有机气溶胶（SOA）在内的深圳市区PM_2.5各种一次和二次来源贡献，本文于2017年9月2日~2018年8月29日在深圳市大学城点位开展PM_2.5样品采集，并进行化学组分和水溶性有机物（WSOM）质谱测量，共获得162组有效数据.观测期间深圳市大气PM_2.5平均质量浓度为26μg/m³，在传统PMF源解析的基础上加入羧基离子碎片（CO₂⁺）作为SOA的示踪物，加入水溶性有机氧（WSOO）用于计算各因子O/C，验证有机物解析效果.结果表明，SOA可以被独立解析出，其O/C明显高于其他一次污染源中有机物；机动车、二次硫酸盐、二次硝酸盐、SOA为最主要的4个源，对PM_2.5质量浓度的贡献分别为25%、23%、17%和10%，船舶、地面扬尘、老化海盐、建筑尘、生物质燃烧、燃煤和工业贡献均在5%以内.各个源的变化特征表明，机动车、二次硫酸盐、二次硝酸盐、SOA等源贡献呈现冬高夏低的季节特征，与冬季季风条件下源自内陆的污染传输密切相关.污染天气时，二次硝酸盐和SOA的贡献增加相对最显著，因此NOx和挥发性有机物是减排的关键.

Abstract

In order to identify the contribution of all primary and secondary sources, including secondary organic aerosol (SOA), of PM_2.5 in the urban area of Shenzhen, PM_2.5 samples were collected continuously from 2nd September, 2017 to 29th August, 2018 at Shenzhen university town. The chemical components of PM_2.5 and mass spectrometry of water-soluble organic matter (WSOM) were measured, with 162 valid datasets obtained. During the observation period, the mean annual mass concentration of PM_2.5 was 26 µg/m³. Based on the experience of traditional source apportionment of PM_2.5, the carboxylic acid ion fragment (CO₂⁺) was added to the PMF model as a tracer of SOA. The water-soluble organic oxygen (WSOO) was also added to the PMF model for the calculation of the O/C of each factor, which was used to verify the apportionment of organic matter. The results show that SOA could be resolved independently, and the O/C was significantly higher than that of the organic matters in primary sources. Vehicle emissions, secondary sulfate, secondary nitrate and SOA were the four main sources, accounting 25%, 23%, 17% and 10% to the mass concentration of PM_2.5, respectively. While ships emissions, fugitive dust, aged sea salt, building dust, biomass burning, coal combustion and industry emissions each contributed less than 5%. The variations of vehicle emissions, secondary sulfate, secondary nitrate and SOA showed higher mass concentrations in winter and lower in summer, which was closely related to the pollution transport from inland under the winter monsoon. The contribution of secondary nitrate and SOA significantly increased during the polluted days, therefore, NO_x and volatile organic compounds were the keys of emission reduction.

导出引用

苏翠平, 孙逸飞, 曹礼明, 王川, 黄晓锋, 何凌燕. 加入SOA示踪的深圳大气PM_2.5受体模型源解析[J]. 中国环境科学. 2020, 40(12): 5124-5132

SU Cui-ping, SUN Yi-fei, CAO Li-ming, WANG Chuan, HUANG Xiao-feng, HE Ling-yan. Source apportionment of PM_2.5 in Shenzhen based on receptor model with SOA tracer[J]. China Environmental Science. 2020, 40(12): 5124-5132

中图分类号： X513

参考文献

[1] Campbell P, Zhang Y, Yan F, et al. Impacts of transportation sector emissions on future US air quality in a changing climate. Part Ⅱ:Air quality projections and the interplay between emissions and climate change[J]. Environmental Pollution, 2018,238:918-903.
[2] Gao M, Saide P E, Xin J, et al. Estimates of Health Impacts and Radiative Forcing in Winter Haze in Eastern China through Constraints of Surface PM_2.5, Predictions[J]. Environmental Science and Technology, 2017,51(4):2178-2185.
[3] Amarloei A, Fazlzadeh M, Jafari, A J, et al. Particulate matters and bioaerosols during Middle East dust storms events in Ilam, Iran[J]. Microchemical Journal, 2020,152:104280.
[4] Puthussery J V, Zhang C, Verma V. Development and field testing of an online instrument for measuring the real-time oxidative potential of ambient particulate matter based on dithiothreitol assay[J]. Atmospheric Measurement Techniques, 2018,11(10):5767-5780.
[5] 唐孝炎,张远航,邵敏.大气环境化学[M]. 北京:高等教育出版社, 2006:268-548. Tang X Y, Zhang Y H, Shao M. Atmospheric environmental chemistry[M]. Beijing:Higher Education Press, 2006:268-548.
[6] Lee S, Liu W, Wang Y, et al. Source Apportionment of PM_2.5:Comparing PMF and CMB results for four ambient monitoring sites in the southeastern United States[J]. Atmospheric environment, 2008, 42(18):4126-4137.
[7] Wang Y, Jia C, Tao J, et al. Chemical characterization and source apportionment of PM_2.5 in a semi-arid and petrochemical-industrialized city, Northwest China[J]. Science of the Total Environment, 2016,573:1031-1040.
[8] Choi J K, Heo J B, Ban S J, et al. Source apportionment of PM_2.5 at the coastal area in Korea[J]. Science of the Total Environment, 2013, 447(1):370-380.
[9] Fan J, Shang Y N, Zhang X J, et al., Joint pollution and source apportionment of PM_2.5 among three different urban environments in Sichuan Basin, China[J]. Science of the Total Environment, 2020, 714:136305.
[10] Guo S, Hu M, Guo Q, et al. Primary sources and secondary formation of organic aerosols in Beijing, China[J]. Environmental Science and Technology, 2012,46:9846-9853.
[11] Ding X, Wang X, Gao B, et al. Tracer-based estimation of secondary organic carbon in the Pearl River Delta, south China[J]. Journal of Geophysical Research:Atmospheres, 2012,117:D05313.
[12] Huang X F, Yun H, Gong Z H, et al. Source apportionment and secondary organic aerosol estimation of PM_2.5 in an urban atmosphere in China[J]. Science China Earth Sciences, 2014,057(6):1352-1362.
[13] Huang, X F, Zou B B, He L Y, et al. Exploration of PM_2.5 sources on the regional scale in the Pearl River Delta based on ME-2modeling[J]. Atmospheric Chemistry and Physics, 2018,11563-11580.
[14] Fortner E, Onasch T, Canagaratna M, et al. Examining the Chemical Composition of Black Carbon Particles from Biomass Burning with SP-AMS[J]. Journal of Aerosol Science, 2018:S0021850217304421.
[15] 郭松,胡敏,尚冬杰,等.基于外场观测的大气二次有机气溶胶研究[J]. 化学学报, 2014,72(2):145-157. Guo S, Hu M, Shang D J, et al. Study on secondary organic aerosols based on field observation[J]. Journal of Chemistry, 2014,72(2):145-157.
[16] 任宇超,邹北冰,朱乔,等.深圳市近年来PM_2.5污染控制效果分析[J]. 环境污染与防治, 2017,39(2):117-121. Ren Y C, Zou B B, Zhu Q, et al. Effects of control measures on Shenzhen PM_2.5 pollution in recent years[J]. Environmental pollution and Prevention, 2017,39(2):117-121.
[17] Cao L M, Huang X F, Li Y Y, et al. Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China[J]. Atmospheric Chemistry and Physics, 2017,18(3):1-21.
[18] 邹北冰.基于ME-2模型珠三角区域大气PM_2.5源解析研究[D]. 北京:北京大学, 2018. Zou B B. Source apportionment of atmospheric PM_2.5 in the Pearl River Delta region based on the ME-2model[D]. Beijing:Peking University, 2018.
[19] Canagaratna M R, Jimenez J L, Kroll J H, et al. Elemental ratio measurements of organic compounds using aerosol mass spectrometry:characterization, improved calibration, and implications[J]. Atmospheric Chemistry and Physics, 2015,15(1):253-272.
[20] Liu B S, Wu J H, Zhang J Y, et al. Characterization and source apportionment of PM_2.5, based on error estimation from EPA PMF 5.0model at a medium city in China[J]. Environmental Pollution, 222:10-22.
[21] Paatero P, Tapper U. Positive matrix factorization:A non-negative factor model with optimal utilization of error estimates of data values[J]. Environmetrics, 1994,5(2):111-126.
[22] 胡伟伟,我国典型大气环境下亚微米有机气溶胶来源与二次转化研究[D]. 北京:北京大学, 2012. Hu W W. Source and secondary conversion of submicron organic aerosols in typical atmospheric environments in China[D]. Beijing:Peking University, 2012
[23] 孙天乐,邹北冰,黄晓锋,等.深圳市大气PM_2.5来源解析[J]. 中国环境科学, 2019,39(1):15-22. Sun T L, Zou B B, Huang X F, et al. Source apportionment of atmospheric PM_2.5 in Shenzhen[J]. Chinese Journal of Environmental Sciences, 2019,39(1):15-22.
[24] 申航印,何凌燕,林理量,等.利用ME-2模型提升PM_2.5源解析效果[J]. 中国环境科学, 2019,39(9):3682-3690. Shen H Y, He L Y, Lin L L, et al. Improved PM_2.5 source apportionment results using the multilinear engine (ME-2) model[J]. China Environmental Science, 2019,39(1):15-22.
[25] Zou B B, Huang X F, Zhang B, et al. Source apportionment of PM_2.5, pollution in an industrial city in southern China[J]. Atmospheric Pollution Research, 2017,8(6):1193-1202.
[26] Yuan Z, Lau A K H, Zhang H, et al. Identification and spatiotemporal variations of dominant PM₁₀ sources over Hong Kong[J]. Atmospheric Environment, 2006,40(10):1803-1815.
[27] Huang X H H, Bian Q, Ng W M, et al. Characterization of PM_2.5 major components and source investigation in suburban Hong Kong:A One Year Monitoring Study[J]. Aerosol and Air Quality Research, 2014,14:237-250.
[28] 林晓辉,赵阳,樊孝俊,等.南昌市秋季大气PM_2.5中金属元素富集特征及来源分析[J]. 环境科学, 2016,37(1):35-40. Lin X H, Zhao Y, Fan X J, et al. Enrichment characteristics and source analysis of metal elements in atmospheric PM_2.5 in Nanchang in autumn[J]. Environmental science, 2016,37(1):35-40.
[29] Hien P D, Binh N T, Truong Y, et al. Comparative receptor modelling study of TSP, PM2, and PM2-10, in Ho Chi Minh City[J]. Atmospheric Environment, 2001,35(15):2669-2678.
[30] Chow J C. Measurement methods to determine compliance with ambient air quality standards for suspended particles[J]. Journal of the Air and Waste Management Association, 1995,45:320-382.
[31] Zabalza J, Ogulei D, Hopke P K. Concentration and Sources of PM₁₀ and its Constituents in Alsasua, Spain[J]. Water Air and Soil Pollution, 2006,174:385-404.
[32] Viana M, Querol X, Alastuey A, et al. Identification of PM sources by principal component analysis (PCA) coupled with wind direction data[J]. Chemosphere, 2006,65(11):2411-2418.
[33] Huang X F, Zhao Q B, He L Y, et al. Identification of secondary organic aerosols based on aerosol mass spectrometry[J]. Science China Chemistry, 2010,53(12):2593-2599.
[34] Querol X, Viana M, Alastuey A. Source origin of trace elements in PM from regional background, urban and industrial sites of Spain[J]. Atmospheric Environment, 2007,41:7219-7231.
[35] 高茂尚,李慧颖,李嫣婷,等.深圳市冬季PM_2.5中水溶性有机物的来源特征[J]. 中国环境科学, 2018,38(11):19-24. Gao M S, Li H Y, Li Y T, et al. Source characteristics of water soluble organic matter in PM_2.5 in Shenzhen in winter[J]. Chinese Journal of Environmental Sciences, 2018,38(11):19-24.
[36] Canagaratna M R, Jimenez J L, Kroll J H, et al. Elemental ratio measurements of organic compounds, using aerosol mass spectrometry:characterization, improved calibration, and implications[J]. Atmospheric Chemistry and Physics, 2015,15(1):253-272.
[37] 朱乔.基于AMS-ME-2的我国东部不同大气环境下有机气溶胶的来源解析[D]. 北京:北京大学, 2019. Zhu Q. Source apportionment of organic aerosols in different atmospheric environments in eastern China based on AMS-ME-2[D]. Beijing:Peking University, 2019.
[38] Elser M, Huang R J, Wolf R, et al. New insights into PM_2.5 chemical composition and sources in two major cities in China during extreme haze events using aerosol mass spectrometry[J]. Atmospheric Chemistry and Physics, 2016,16(5):3207-3225.
[39] Zhu Q, Huang X, Cao L, et al. Improved source apportionment of organic aerosols in complex urban air pollution using the multilinear engine (ME-2)[J]. Atmospheric Measurement Techniques, 2018,11(2):1049-1060.