广州近郊秋季大气有机气溶胶来源及特征组分

廖芸仟, 余淼, 梁琳, 王小月, 尹健帆, 房泽, 常鸣, 袁斌, 邵敏, 黄山

中国环境科学 ›› 2026, Vol. 46 ›› Issue (1) : 53-65.

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中国环境科学 ›› 2026, Vol. 46 ›› Issue (1) : 53-65.
大气污染与控制

广州近郊秋季大气有机气溶胶来源及特征组分

  • 廖芸仟, 余淼, 梁琳, 王小月, 尹健帆, 房泽, 常鸣, 袁斌, 邵敏, 黄山
作者信息 +

Sources and characteristic components of atmospheric organic aerosols in the autumn suburbs of Guangzhou

  • LIAO Yun-qian, YU Miao, LIANG Lin, WANG Xiao-yue, YIN Jian-fan, FANG Ze, CHANG Ming, YUAN Bin, SHAO Min, HUANG Shan
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文章历史 +

摘要

于2022年秋季利用黑碳-气溶胶质谱仪(SP-AMS)对广州近郊大气PM1进行了两个月观测.基于正交矩阵因子分析法(PMF)对有机气溶胶(OA)进行来源解析,并对其特征组分颗粒态有机硝酸酯(pON)进行量化讨论.观测期间PM1[(15.90 ± 12.28)μg/m3]受有机物主导(57.8%),除硫酸盐外主要组分呈现夜高日低的特征.OA主要来源于本地二次生成(28.3%)和长距离传输(23.9%),及烹饪、机动车尾气、生物质燃烧等一次排放(47.8%).pON对OA贡献可达24.7%,且在总硝酸盐浓度低时占比显著升高.其夜间增加可促进次日大气氧化性升高.pON主要源于本地二次生成(51.5%)和机动车尾气(39.8%).高颗粒物浓度时段OA受本地二次生成和机动车排放主导;高臭氧浓度时段,有机物及硫酸盐出现明显中午峰(光化学氧化作用),二次OA贡献升至59.8%,pON也主要源于本地二次生成(60.8%).

Abstract

A two-month observation of atmospheric PM1 in suburban Guangzhou in autumn 2022 was conducted using a Soot-Particle High Resolution Time-of-Flight Aerosol Mass Spectrometer (SP-AMS). Sources apportionment of organic aerosol (OA) was performed using Positive Matrix Factorization (PMF). OA’s characteristic component particulate organic nitrates (pON) were quantified and explored. During the observation period, PM[ (15.90 ± 12.28) μg/m3] was dominated by organics (57.8%), with major components (excluding sulfate) exhibiting higher nocturnal concentrations than diurnal concentrations. OA was mainly contributedby local secondary formation (28.3%), long-range transport (23.9%), and primary emissions such as cooking, vehicle exhaust, and biomass burning (collectively 47.8%). pON contributed significantly to OA (24.7%), increasing markedly under low total nitrate concentrations. Its nocturnal increase may enhance next-day atmospheric oxidation capacity. pON mainly derived from local secondary formation (51.5%) and vehicle exhaust (39.8%). During high PM events, OA was dominated by local secondary formation and vehicle emissions; during high ozone conditions, organics and sulfate showed pronounced midday peaks (photochemical oxidation), secondary OA contribution rose to 59.8%, and pON was primarily from local secondary formation (60.8%).

关键词

亚微米级颗粒物(PM1) / 有机气溶胶 / 来源解析 / 有机硝酸酯 / 气溶胶质谱(AMS)

Key words

submicron particles (PM1) / organic aerosol / source apportionment / organic nitrates / Aerosol Mass Spectrometry (AMS)

引用本文

导出引用
廖芸仟, 余淼, 梁琳, 王小月, 尹健帆, 房泽, 常鸣, 袁斌, 邵敏, 黄山. 广州近郊秋季大气有机气溶胶来源及特征组分[J]. 中国环境科学. 2026, 46(1): 53-65
LIAO Yun-qian, YU Miao, LIANG Lin, WANG Xiao-yue, YIN Jian-fan, FANG Ze, CHANG Ming, YUAN Bin, SHAO Min, HUANG Shan. Sources and characteristic components of atmospheric organic aerosols in the autumn suburbs of Guangzhou[J]. China Environmental Science. 2026, 46(1): 53-65
中图分类号: X511   

参考文献

[1] Molina L T, Gallardo L, Andrade M, et al. Pollution and its impacts on the South American cryosphere[J]. Earth's Future, 2015,3(12):345- 369.
[2] Fenger J. Urban air quality[J]. Atmospheric Environment, 1999, 33(29):4877-4900.
[3] Beelen R, Raaschou-Nielsen O, Stafoggia M, et al. Effects of long- term exposure to air pollution on natural-cause mortality: an analysis of 22European cohorts within the multicentre ESCAPE project[J]. Lancet, 2014,383(9919):785-795.
[4] Gunthe S S, Liu P, Panda U, et al. Enhanced aerosol particle growth sustained by high continental chlorine emission in India[J]. Nature Geoscience, 2021,14(2):77-84.
[5] Kuang Y, Huang S, Xue B, et al. Contrasting effects of secondary organic aerosol formations on organic aerosol hygroscopicity[J]. Atmospheric Chemistry and Physics, 2021,21(13):10375-10391.
[6] Zhou W, Xu W, Kim H, et al. A review of aerosol chemistry in Asia: insights from aerosol mass spectrometer measurements[J]. Environmental Science: Processes & Impacts, 2020,22(8):1616-1653.
[7] Sun Y, Du W, Fu P, et al. Primary and secondary aerosols in Beijing in winter: sources, variations and processes[J]. Atmospheric Chemistry and Physics, 2016,16(13):8309-8329.
[8] Hu W, Hu M, Hu W, et al. Chemical composition, sources, and aging process of submicron aerosols in Beijing: Contrast between summer and winter[J]. Journal of Geophysical Research: Atmospheres, 2016, 121(4):1955-1977.
[9] Zhang Q, Alfarra M R, Worsnop D R, et al. Deconvolution and quantification of hydrocarbon-like and oxygenated organic aerosols based on aerosol mass spectrometry[J]. Environmental science & technology, 2005,39(13):4938-4952.
[10] Alfarra M R, Prevot A S, Szidat S, et al. Identification of the mass spectral signature of organic aerosols from wood burning emissions[J]. Environmental science & technology, 2007,41(16):5770-5777.
[11] Tang C, Zhang X, Tian P, et al. Chemical characteristics and regional transport of submicron particulate matter at a suburban site near Lanzhou, China[J]. Environmental Research, 2022,212,113179.
[12] Li H, Zhang Q, Zheng B, et al. Nitrate-driven urban haze pollution during summertime over the North China Plain[J]. Atmospheric Chemistry and Physics, 2018,18(8):5293-5306.
[13] Wen L, Xue L, Wang X, et al. Summertime fine particulate nitrate pollution in the North China Plain: increasing trends, formation mechanisms and implications for control policy[J]. Atmospheric Chemistry and Physics, 2018,18(15):11261-11275.
[14] Zhou W, Gao M, He Y, et al. Response of aerosol chemistry to clean air action in Beijing, China: Insights from two-year ACSM measurements and model simulations[J]. Environmental Pollution, 2019,255,113345.
[15] Zhou S, Collier S, Xu J, et al. Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.[J]. Journal of Geophysical Research: Atmospheres, 2016,121(10):6049-6065.
[16] Day D A, Campuzano-Jost P, Nault B A, et al. A systematic re-evaluation of methods for quantification of bulk particle-phase organic nitrates using real-time aerosol mass spectrometry[J]. Atmospheric Measurement Techniques, 2022,15(2):459-483.
[17] 于广河,曹礼明,朱乔,等,深圳大气有机硝酸酯粒径分布特征和来源研究[J]. 中国环境科学, 2022,42(4):1510-1517. Yu G H, Cao L M, Zhu Q, et al. Sizing and source characterization of particulate organic nitrates based on long time-of-flight aerosol mass spectrometer (Long-ToF-AMS) in Shenzhen[J]. China Environmental Science, 2022,42(4):1510-1517.
[18] Fry J, Draper D, Zarzana K, et al. Observations of gas-and aerosol-phase organic nitrates at BEACHON-RoMBAS 2011[J]. Atmospheric Chemistry and Physics, 2013,13(17):8585-8605.
[19] Kenagy H S, Romer Present P S, Wooldridge P J, et al. Contribution of organic nitrates to organic aerosol over South Korea during KORUS- AQ[J]. Environmental science & technology, 2021,55(24):16326- 16338.
[20] Rollins A W, Browne E C, Min K E, et al. Evidence for NOx control over nighttime SOA formation[J]. Science, 2012, 337(6099):1210- 1212.
[21] Xu L, Suresh S, Guo H, et al. Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates[J]. Atmospheric Chemistry and Physics, 2015,15(13):7307-7336.
[22] Yu K, Zhu Q, Du K, et al. Characterization of nighttime formation of particulate organic nitrates based on high-resolution aerosol mass spectrometry in an urban atmosphere in China[J]. Atmospheric Chemistry and Physics, 2019,19(7):5235-5249.
[23] Kiendler‐Scharr A, Mensah A A, Friese E, et al. Ubiquity of organic nitrates from nighttime chemistry in the European submicron aerosol[J]. Geophysical Research Letters, 2016,43(14):7735-7744.
[24] Horowitz L W, Liang J, Gardner G M, et al. Export of reactive nitrogen from North America during summertime: Sensitivity to hydrocarbon chemistry[J]. Journal of Geophysical Research: Atmospheres, 1998,103(D11):13451-13476.
[25] Lee B H, Mohr C, Lopez-Hilfiker F D, et al. Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets[J]. Proceedings of the National Academy of Sciences, 2016,113(6):1516- 1521.
[26] Farmer D, Matsunaga A, Docherty K, et al. Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry[J]. Proceedings of the National Academy of Sciences, 2010,107(15):6670-6675.
[27] Farmer D, Perring A, Wooldridge P, et al. Impact of organic nitrates on urban ozone production[J]. Atmospheric Chemistry and Physics, 2011,11(9):4085-4094.
[28] Li C, Chen X, Wang H, et al. The impact of organic nitrates on summer ozone formation in Shanghai, China[J]. Atmospheric Chemistry and Physics, 2025,25(7):3905-3918.
[29] Perring A, Pusede S, Cohen R C. An observational perspective on the atmospheric impacts of alkyl and multifunctional nitrates on ozone and secondary organic aerosol[J]. Chemical reviews, 2013,113(8):5848- 5870.
[30] Wang Y, Takeuchi M, Wang S, et al. Photolysis of gas-phase atmospherically relevant monoterpene-derived organic nitrates[J]. The Journal of Physical Chemistry A, 2023,127(4):987-999.
[31] 李伟,黄山,袁斌,等,大气颗粒态有机硝酸酯的转化机制、测量技术及应用[J]. 中国环境科学, 2021,41(7):3017-3028. Li W, Huang S, Yuan B, et al. Mechanism, measurement techniques and their application for particulate organonitrates[J]. China Environmental Science, 2021,41(7):3017-3028.
[32] Zhai M, Kuang Y, Liu L, et al. Insights into characteristics and formation mechanisms of secondary organic aerosols in the Guangzhou urban area[J]. Atmospheric Chemistry and Physics, 2023, 23(9):5119-5133.
[33] Liu T, Zhou L, Liu Q, et al. Secondary organic aerosol formation from urban roadside air in Hong Kong[J]. Environmental science & technology, 2019,53(6):3001-3009.
[34] 李孟林,朱乔,曹礼明,等.深圳秋季大气有机气溶胶来源与挥发性研究[J]. 中国环境科学, 2021,41(9):4009-4015. Li M L, Zhu Q, Cao L M, et al. Sources and volatility of atmospheric organic aerosol in autumn in Shenzhen[J]. China Environmental Science, 2021,41(9):4009-4015.
[35] 伍莉娜.基于SP-AMS测量的珠三角城乡大气颗粒态有机硝酸酯生成机制及影响因素研究[D]. 广州:暨南大学, 2023. Wu L N. Atmospheric formation and its influence factors of particulate organonitrate in urban and rural PRD based on SP-AMS measurements[D]. Guangzhou: Jinan University, 2023.
[36] Canagaratna M, Jayne J, Jimenez J, et al. Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer[J]. Mass Spectrometry Reviews, 2007,26(2):185-222.
[37] Onasch T, Trimborn A, Fortner E, et al. Soot particle aerosol mass spectrometer: development, validation, and initial application[J]. Aerosol Science and Technology, 2012,46(7):804-817.
[38] Middlebrook A M, Bahreini R, Jimenez J L, et al. Evaluation of composition-dependent collection efficiencies for the aerodyne aerosol mass spectrometer using field data[J]. Aerosol Science and Technology, 2012,46(3):258-271.
[39] Paatero P. Least squares formulation of robust non-negative factor analysis[J]. Chemometrics and Intelligent Laboratory systems, 1997, 37(1):23-35.
[40] Ulbrich I, Canagaratna M, Zhang Q, et al. Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data[J]. Atmospheric Chemistry and Physics, 2009,9(9): 2891-2918.
[41] Zhang Q, Jimenez J L, Canagaratna M R, et al. Understanding atmospheric organic aerosols via factor analysis of aerosol mass spectrometry: A review[J]. Analytical and Bioanalytical Chemistry, 2011,401(10):3045-3067.
[42] Lanz V, Alfarra M, Baltensperger U, et al. Source apportionment of submicron organic aerosols at an urban site by factor analytical modelling of aerosol mass spectra[J]. Atmospheric Chemistry and Physics, 2007,7(6):1503-1522.
[43] Chen G, Morawska L, Zhang W, et al. Spatiotemporal variation of PM1 pollution in China[J]. Atmospheric Environment, 2018,178:198-205.
[44] Sun Y, Wang Z, Du W, et al. Long-term real-time measurements of aerosol particle composition in Beijing, China: seasonal variations, meteorological effects, and source analysis[J]. Atmospheric Chemistry and Physics, 2015,15(17):10149-10165.
[45] Shah V, Jaeglé L, Thornton J A, et al. Chemical feedbacks weaken the wintertime response of particulate sulfate and nitrate to emissions reductions over the eastern United States[J]. Proceedings of the National Academy of Sciences, 2018,115(32):8110-8115.
[46] Li J, Liu Z, Gao W, et al. Insight into the formation and evolution of secondary organic aerosol in the megacity of Beijing, China[J]. Atmospheric Environment, 2020,220,117070.
[47] Xie Y, Wang G, Wang X, et al. Nitrate-dominated PM2.5 and elevation of particle pH observed in urban Beijing during the winter of 2017[J]. Atmospheric Chemistry and Physics, 2020,20(8):5019-5033.
[48] Liu Y, Wu L, Huang S, et al. Sources, size-resolved deposition in the human respiratory tract and health risks of submicron black carbon in urban atmosphere in pearl river delta, China[J]. Science of the Total Environment, 2023,891,164391.
[49] Rivellini L H, Adam M G, Kasthuriarachchi N, et al. Characterization of carbonaceous aerosols in Singapore: insight from black carbon fragments and trace metal ions detected by a soot particle aerosol mass spectrometer[J]. Atmospheric Chemistry and Physics, 2020,20(10): 5977-5993.
[50] Saarikoski S, Niemi J V, Aurela M, et al. Sources of black carbon at residential and traffic environments obtained by two source apportionment methods[J]. Atmospheric Chemistry and Physics, 2021, 21(19):14851-14869.
[51] Henry R, Norris G A, Vedantham R, et al. Source region identification using kernel smoothing[J]. Environmental science & technology, 2009,43(11):4090-4097.
[52] Huang R J, He Y, Duan J, et al. Contrasting sources and processes of particulate species in haze days with low and high relative humidity in wintertime Beijing[J]. Atmospheric Chemistry and Physics, 2020, 20(14):9101-9114.
[53] 王浩飞,刘立忠,刘焕武,等.西安南郊夏季颗粒物组成分类、理化特征及潜在来源[J]. 环境工程学报, 2025,19(1):188-200. Wang H F, Liu L Z, Liu H W, et al. Composition classification, physicochemical characteristics and potentialsources of particulate matter in the southern suburbs of Xi 'an in summer[J]. Chinese Journal of Environmental Engineering, 2025,19(1):188-200.
[54] Mohr C, DeCarlo P F, Heringa M F, et al. Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data[J]. Atmospheric Chemistry and Physics, 2012,12(4):1649-1665.
[55] Crippa M, El Haddad I, Slowik J G, et al. Identification of marine and continental aerosol sources in Paris using high resolution aerosol mass spectrometry[J]. Journal of Geophysical Research: Atmospheres, 2013,118(4):1950-1963.
[56] Qin Y M, Tan H B, Li Y J, et al. Impacts of traffic emissions on atmospheric particulate nitrate and organics at a downwind site on the periphery of Guangzhou, China[J]. Atmospheric Chemistry and Physics, 2017,17(17):10245-10258.
[57] Hu W W, Hu M, Yuan B, et al. Insights on organic aerosol aging and the influence of coal combustion at a regional receptor site of central eastern China[J]. Atmospheric Chemistry and Physics, 2013,13(19): 10095-10112.
[58] Aiken A C, Salcedo D, Cubison M J, et al. Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0)–Part 1: Fine particle composition and organic source apportionment[J]. Atmospheric Chemistry and Physics, 2009,9(17):6633-6653.
[59] Saarikoski S, Carbone S, Decesari S, et al. Chemical characterization of springtime submicrometer aerosol in Po Valley, Italy[J]. Atmospheric Chemistry and Physics, 2012,12(18):8401-8421.
[60] Sun Y L, Zhang Q, Schwab J, et al. Characterization of the sources and processes of organic and inorganic aerosols in New York city with a high-resolution time-of-flight aerosol mass spectrometer[J]. Atmospheric Chemistry and Physics, 2011,11(4):1581-1602.
[61] Bottenus C L, Massoli P, Sueper D, et al. Identification of amines in wintertime ambient particulate material using high resolution aerosol mass spectrometry[J]. Atmospheric Environment, 2018,180:173-183.
[62] Zhu W, Shi J, Guo S, et al. Comparative analysis of methods for seasonal particulate organic nitrate estimation in urban areas[J]. npj Climate and Atmospheric Science, 2025,8(1):21.
[63] Hayes P, Ortega A, Cubison M, et al. Organic aerosol composition and sources in Pasadena, California, during the 2010 CalNex campaign[J]. Journal of Geophysical Research: Atmospheres, 2013,118(16):9233- 9257.
[64] Graeffe F, Heikkinen L, Garmash O, et al. Detecting and characterizing particulate organic nitrates with an aerodyne long-ToF aerosol mass spectrometer[J]. ACS Earth and Space Chemistry, 2022,7(1):230-242.
[65] Ge D, Nie W, Sun P, et al. Characterization of particulate organic nitrates in the Yangtze River Delta, East China, using the time-of- flight aerosol chemical speciation monitor[J]. Atmospheric Environment, 2022,272,118927.
[66] Huang W, Yang Y, Wang Y, et al. Exploring the inorganic and organic nitrate aerosol formation regimes at a suburban site on the North China Plain[J]. Science of the Total Environment, 2021,768,144538.
[67] Zhu Q, Cao L M, Tang M X, et al. Characterization of organic aerosol at a rural site in the North China Plain region: Sources, volatility and organonitrates[J]. Advances in Atmospheric Sciences, 2021,38(7): 1115-1127.
[68] Xu W, Sun Y, Wang Q, et al. Seasonal characterization of organic nitrogen in atmospheric aerosols using high resolution aerosol mass spectrometry in Beijing, China[J]. ACS Earth and Space Chemistry, 2017,1(10):673-682.

基金

国家重点研发计划项目(2023YFC3706204);国家自然科学基金项目(42377088,41807302);广东省佛山生态环境监测站项目(GZGK24P047C0239Z);广东省科技计划项目(2024B1212080002)

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