光化学氧化对深圳市含黑碳气溶胶混合态和光吸收的影响

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摘要于2021年2月在深圳开展了含黑碳气溶胶混合态和光学性质的测量,结合奇氧数(O_x)的同步分析,以探究光化学氧化对城市大气中含黑碳气溶胶包裹物、形貌与光吸收能力的影响.结果表明:观测期间黑碳颗粒群平均相对包裹物量(包裹物与黑碳核质量比,M_R)平均值为4.3±0.7,有效密度平均值为(1.35±0.10) g/cm³,整体颗粒群形貌为球形的观测时段占比为70 %,表明深圳城市点含黑碳气溶胶主要为中等不规则形貌的内部混合态颗粒.光化学氧化在含黑碳气溶胶混合态演变过程中起到重要作用.随着O_x的增加,颗粒群平均M_R增幅约为38 %,平均有效密度从1.32g/cm³增至1.44g/cm³,动力学形状因子从1.05递减至1.00,表明光化学氧化过程促使非黑碳组分累积并使颗粒趋向于形成更致密的核壳球形.此外,O_x增加过程中,吸光增强(E_abs)增幅约为20%,增长速率为0.002/10^-9,表明光化学氧化对城市点含黑碳气溶胶光吸收起到关键的驱动作用.

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	彭妍
	林晓玉
	谢婷婷
	魏静
	李征宇
	何凌燕
	黄晓锋

关键词 ：光化学氧化, 含黑碳气溶胶, 混合态, 吸光性

Abstract：In February 2021, we conducted a study in Shenzhen to measure the mixing state and optical properties of black carbon (BC)-containing aerosols. Simultaneously, we analyzed odd oxygen (O_x) to explore the effects of photochemical oxidation on coating, morphology, and light absorption of BC-containing aerosols in an urban environment. The results show that, during the observation period, the mean bulk-averaged relative coating amounts (coating-to-core mass ratio, M_R) over particle population was 4.3 ±0.7. The mean effective density was (1.35 ±0.10) g/cm³, and about 70% of the observed period exhibited spherical morphology, indicating that the BC-containing aerosols in Shenzhen were predominantly composed of internally mixed particles with moderately irregular shapes. Photochemical oxidation played an important role in the mixing state evolution of BC-containing aerosols. With rising O_x concentrations, the bulk-averaged M_R increased by about 38%, the effective density increased from 1.32g/cm³ to 1.44g/cm³, and the dynamic shape factor decreased from 1.05 to 1.00, indicating that the photochemical oxidation process resulted in the accumulation of non-BC components and reshaped more compact spherical particles with core-shell structure. Additionally, as O_x concentrations increased, the light absorption enhancement (E_abs) exhibited an approximately 20% increase, with a growth rate of 0.002/ppbv, suggesting the key role of photochemical oxidation in enhancing light absorption of BC-containing aerosols in an urban site.

Key words： photochemical oxidation BC-containing aerosols mixing state light absorption

收稿日期: 2023-11-18

PACS:

X703.5

基金资助:深圳市科技计划资助项目(JCYJ20200109120401943)

通讯作者: 黄晓锋,教授,huangxf@pku.edu.cn E-mail: huangxf@pku.edu.cn

作者简介: 彭妍(1997-),女,山东滨州人,北京大学博士研究生,主要从事黑碳气溶胶混合态及气候效应研究.发表论文8篇.pengyan@pku.edu.cn.

引用本文:

彭妍, 林晓玉, 谢婷婷, 魏静, 李征宇, 何凌燕, 黄晓锋. 光化学氧化对深圳市含黑碳气溶胶混合态和光吸收的影响[J]. 中国环境科学, 2024, 44(6): 2970-2976. PENG Yan, LIN Xiao-yu, XIE Ting-ting, WEI Jing, LI Zheng-yu, HE Ling-yan, HUANG Xiao-feng. Effects of photochemical oxidation on the mixing state and light absorption of black carbon-containing aerosols in Shenzhen. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(6): 2970-2976.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2024/V44/I6/2970

[1] Bond T C, Doherty S J, Fahey D W, et al. Bounding the role of black carbon in the climate system:A scientific assessment[J]. Journal of Geophysical Research. Atmospheres, 2013,118:5380-5552.
[2] Zhang Y, Zhang Q, Wu N, et al. Weakened haze mitigation induced by enhanced aging of black carbon in China[J]. Environmental Science&Technology, 2022,56:7629-7636.
[3] Ding A J, Huang X, Nie W, et al. Enhanced haze pollution by black carbon in megacities in China[J]. Geophysical Research Letters, 2016, 43:2873-2879.
[4] China S, Mazzoleni C, Gorkowski K, et al. Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles[J]. Nature Communications, 2013,4:2122-2122.
[5] Adachi K, Chung S H,Buseck P R. Shapes of soot aerosol particles and implications for their effects on climate[J]. Journal of Geophysical Research:Atmospheres, 2010,115:D15206.
[6] Tan T, Guo S, Wu Z, et al. Impact of aging process on atmospheric black carbon aerosol properties and climate effects[J]. Chinese Science Bulletin, 2020,65:4235-4250.
[7] Cappa C D, Onasch T B, Kolesar K R, et al. Radiative absorption enhancements due to the mixing state of atmospheric black carbon[J]. Science, 2012,337:1078-1081.
[8] Liu S, Aiken A C, Gorkowski K, et al. Enhanced light absorption by mixed source black and brown carbon particles in UK winter[J]. Nature Communications, 2015,6:8435-8435.
[9] Peng J, Hu M, Guo S, et al. Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments[J]. Proceedings of the National Academy of Sciences, 2016,113:4266-4271.
[10] Guo S, Hu M, Lin Y, et al. OH-initiated oxidation of m-Xylene on black carbon aging[J]. Environmental Science&Technology, 2016, 50:8605-8612.
[11] Jacobson M Z. Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols[J]. Nature, 2001,409:695-697.
[12] Liu D, Whitehead J, Alfarra M R, et al. Black-carbon absorption enhancement in the atmosphere determined by particle mixing state[J]. Nature Geoscience, 2017,10:184-188.
[13] Cappa C D, Zhang X, Russell L M, et al. Light absorption by ambient black and brown carbon and its dependence on black carbon coating state for two California, USA, cities in winter and summer[J]. Journal of Geophysical Research. Atmospheres, 2019,124:1550-1577.
[14] Zhai J, Yang X, Li L, et al. Absorption enhancement of black carbon aerosols constrained by mixing-state heterogeneity[J]. Environmental Science&Technology, 2022,56:1586-1593.
[15] Wei J, Niu Y-B, Tang M-X, et al. Characterizing formation mechanisms of secondary aerosols on black carbon in a megacity in South China[J]. Science of the Total Environment, 2023,859:160290-160290.
[16] Peng J, Hu M, Guo S, et al. Ageing and hygroscopicity variation of black carbon particles in Beijing measured by a quasi-atmospheric aerosol evolution study (QUALITY) chamber[J]. Atmospheric Chemistry and Physics, 2017,17:10333-10348.
[17] Sun J Y, Wu C, Wu D, et al. Amplification of black carbon light absorption induced by atmospheric aging:temporal variation at seasonal and diel scales in urban Guangzhou[J]. Atmospheric Chemistry and Physics, 2020,20:2445-2470.
[18] Wang Q, Huang R, Zhao Z, et al. Effects of photochemical oxidation on the mixing state and light absorption of black carbon in the urban atmosphere of China[J]. Environmental Research Letters, 2017,12:44012.
[19] Wang T, Zhao G, Tan T, et al. Effects of biomass burning and photochemical oxidation on the black carbon mixing state and light absorption in summer season[J]. Atmospheric Environment, 2021,248:118230.
[20] Schwarz J P, Gao R S, Fahey D W, et al. Single-particle measurements of midlatitude black carbon and light-scattering aerosols from the boundary layer to the lower stratosphere[J]. Journal of Geophysical Research, 2006,111:D16207.
[21] Moteki N, Kondo Y, Nakamura S-i. Method to measure refractive indices of small nonspherical particles:Application to black carbon particles[J]. Journal of Aerosol Science, 2010,41:513-521.
[22] Stolzenburg M R, McMurry P H. Equations governing single and tandem DMA configurations and a new lognormal approximation to the transfer function[J]. Aerosol Science and Technology, 2008,42:421-432.
[23] Peng Y, Cao L-M, Wei J, et al. Key drivers to heterogeneity evolution of black carbon-containing particles in real atmosphere[J]. Science of the Total Environment, 2023,897:166394.
[24] Zhao G, Zhao W, Zhao C. Method to measure the size-resolved real part of aerosol refractive index using differential mobility analyzer in tandem with single-particle soot photometer[J]. Atmospheric Measurement Techniques, 2019,12:3541-3550.
[25] Onasch T B, Trimborn A, Fortner E C, et al. Soot particle aerosol mass spectrometer:development, validation, and initial application[J]. Aerosol Science and Technology, 2012,46:804-817.
[26] Kim J H, Mulholland G W, Kukuck S R, et al. Slip correction measurements of certified PSL nanoparticles using a nanometer differential mobility analyzer (Nano-DMA) for knudsen number from 0.5 to 83[J]. Journal of Research of The National Institute of Standards and Technology, 2005,110:31-54.
[27] Flowers B A, Dubey M K, Mazzoleni C, et al. Optical-chemical-microphysical relationships and closure studies for mixed carbonaceous aerosols observed at Jeju Island; 3-laser photoacoustic spectrometer, particle sizing, and filter analysis[J]. Atmospheric Chemistry and Physics, 2010,10:10387-10398.
[28] Liu D, Allan J D, Young D E, et al. Size distribution, mixing state and source apportionment of black carbon aerosol in London during wintertime[J]. Atmospheric Chemistry and Physics, 2014,14:10061-10084.
[29] Zhang Y, Zhang Q, Yao Z, et al. Particle size and mixing state of freshly emitted black carbon from different vombustion sources in China[J]. Environmental Science&Technology, 2020,54:7766-7774.
[30] Ma Y, Huang C, Jabbour H, et al. Mixing state and light absorption enhancement of black carbon aerosols in summertime Nanjing, China[J]. Atmospheric Environment, 2020,222:117141.
[31] Yu C, Liu D, Broda K, et al. Characterising mass-resolved mixing state of black carbon in Beijing using a morphology-independent measurement method[J]. Atmospheric Chemistry and Physics, 2020, 20:3645-3661.
[32] Zhang R, Khalizov A F, Pagels J, et al. Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing[J]. Proceedings of the National Academy of Sciences, 2008,105:10291-10296.
[33] Liu H, Pan X, Wu Y, et al. Effective densities of soot particles and their relationships with the mixing state at an urban site in the Beijing megacity in the winter of 2018[J]. AtmosphericCchemistry and Physics, 2019,19:14791-14804.
[34] Zhang Y, Favez O, Canonaco F, et al. Evidence of major secondary organic aerosol contribution to lensing effect black carbon absorption enhancement[J]. NPJ Climate and Atmospheric Science, 2018,1:47.
[35] Liu H, Pan X, Liu D, et al. Mixing characteristics of refractory black carbon aerosols at an urban site in Beijing[J]. Atmospheric Chemistry and Physics, 2020,20:5771-5785.
[36] Xu J, Wang Q, Deng C, et al. Insights into the characteristics and sources of primary and secondary organic carbon:High time resolution observation in urban Shanghai[J]. Environmental Pollution, 2018,233:1177-1187.
[37] Krasowsky T S, McMeeking G R, Wang D, et al. Measurements of the impact of atmospheric aging on physical and optical properties of ambient black carbon particles in Los Angeles[J]. Atmospheric Environment, 2016,142:496-504.
[38] Knox A, Evans G J, Brook J R, et al. Mass absorption cross-section of ambient black carbon aerosol in relation to chemical age[J]. Aerosol Science and Technology, 2009,43:522-532.