不同季节人为氯排放对二次气溶胶影响的数值模拟

Abstract
Figure/Table
References
Related Citation (15)

Download: PDF (5258 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract Chlorine-containing species released from anthropogenic sources can participate in atmospheric chemical reactions and have an important impact on the formation of secondary aerosols. However, there are few studies on its contribution to the concentration of secondary aerosols in eastern China. In this study, we quantified effects of anthropogenic chlorine emissions on secondary inorganic and organic aerosols in different seasons using the WRF-CMAQ model. The results show that anthropogenic chlorine emissions had much stronger effect on nitrates than on sulfates. Particulate Cl^- could react with HNO₃, N₂O₅, NO₃ and NO₂ to form nitrates, and NH₃ could be converted to ammonium. In winter, spring, summer and autumn, the anthropogenic chlorine emissions elevated both the monthly mean nitrate concentrations by up to 9.8μg/m³ (34.3%), 1.5μg/m³(11.4%), 1.3μg/m³(9.1%), and 2.6μg/m³(10.3%), respectively, and the monthly mean ammonium concentrations by up to 3.0μg/m³ (30.7%), 0.6μg/m³ (10.3%), 0.5μg/m³ (6.5%), and 1.1μg/m³ (8.0%), respectively. This impact was the most significant in winter, while the least in summer. Anthropogenic chlorine emissions have enhanced the degradation of VOCs by Cl atoms and OH radicals. The concentrations of different types of SOA have increased slightly, and the increase in SOA concentration was up to about 6%. The increase in secondary inorganic aerosols and secondary organic aerosols has led to an increase in the total amount of particulate matter. In winter, spring, summer and autumn, the anthropogenic chlorine emissions increased the monthly mean PM₁₀ concentrations by up to 14.0μg/m³(18.3%), 2.5μg/m³(3.0%), 1.9μg/m³(2.8%), and 4.5μg/m³(4.3%), respectively, and also elevated the monthly mean PM_2.5 concentrations by up to 15.0μg/m³(24.4%), 2.1μg/m³(3.5%), 1.2μg/m³(3.2%), and 3.9μg/m³(4.4%), respectively. Such impacts from large to small were winter, autumn, spring and summer and greater in the inland areas than in the coastal areas.

Key words： HCl Cl₂ secondary aerosol CMAQ PM_2.5

Received: 10 January 2022

PACS:

X513

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	LIU Yi-ming
	ZHOU Hui-xian
	LI Si-ting
	SHEN Ao
	FAN Qi

Cite this article:

LIU Yi-ming,ZHOU Hui-xian,LI Si-ting等. Numerical simulation of impacts of anthropogenic chlorine emissions on secondary aerosols in different seasons[J]. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(9): 4059-4072.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2022/V42/I9/4059

[1]	洪莹莹,翁佳烽,谭浩波,等.珠江三角洲秋季典型O3污染的气象条件及贡献量化 [J]. 中国环境科学, 2021,41(1):1-10. Hong Y Y, Wen J F, Tan H B, et al. Meteorological conditions and contribution quantification of typical ozone pollution during autumn in Pearl River Delta [J]. China Environmental Science, 2021,41(1):1-10.
[2]	卫菲菲,刘昊,陆晓波,等.南京市大气细颗粒物二次组分的时空变化特征 [J]. 中国环境科学, 2017,37(8):2866-2876. Wei F F, Liu H, Lu X B, et al. Temporal and spatial characteristics of secondary components of PM2.5 in Nanjing [J]. China Environmental Science, 2017,37(8):2866-2876.
[3]	Zhang Q, Zheng Y X, Tong D, et al. Drivers of improved PM2.5 air quality in China from 2013 to 2017 [J]. Proceedings of the National Academy of Sciences, 2019,116(49):24463-24469.
[4]	Liu Y M, Wang T. Worsening urban ozone pollution in China from 2013 to 2017 – Part 1: The complex and varying roles of meteorology [J]. Atmospheric Chemistry and Physics, 2020,20(11):6305-6321.
[5]	Huang X, Ding A J, Gao J, et al. Enhanced secondary pollution offset reduction of primary emissions during COVID-19lockdown in China [J]. National Science Review, 2021,8(2): nwaa137.
[6]	贾佳,韩力慧,程水源,等.京津冀区域PM2.5及二次无机组分污染特征研究 [J]. 中国环境科学, 2018,38(3):801-811. Jia J, Han L H, Cheng S Y, et al. Pollution characteristic of PM2.5 and secondary inorganic ions in Beijing-Tianjin-Hebei region [J]. China Environmental Science, 2018,38(3):801-811.
[7]	Faxon C B, Allen D T. Chlorine chemistry in urban atmospheres: a review [J]. Environmental Chemistry, 2013,10(3):221-233.
[8]	Thornton J A, Kercher J P, Riedel T P, et al. A large atomic chlorine source inferred from mid-continental reactive nitrogen chemistry [J]. Nature, 2010,464(7286):271-274.
[9]	Fountoukis C, Nenes A. ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K+-Ca2+-Mg2+-NH4+-Na+- SO42--NO3--Cl--H2O aerosols [J]. Atmospheric Chemistry and Physics, 2007,7(17):4639-4659.
[10]	Bertram T H, Thornton J A. Toward a general parameterization of N2O5 reactivity on aqueous particles: the competing effects of particle liquid water, nitrate and chloride [J]. Atmospheric Chemistry and Physics, 2009,9(21):8351-8363.
[11]	Gershenzon M Y, Il'in S, Fedotov N G, et al. The Mechanism of Reactive NO3 Uptake on Dry NaX (X=Cl, Br) [J]. Journal of Atmospheric Chemistry, 1999,34(1):119-135.
[12]	Weis D D, Ewing G E. The reaction of nitrogen dioxide with sea salt aerosol [J]. The Journal of Physical Chemistry A, 1999,103(25):4865- 4873.
[13]	Fu X, Wang T, Wang S X, et al. Anthropogenic emissions of hydrogen chloride and fine particulate chloride in China [J]. Environmental Science & Technology, 2018,52(3):1644-1654.
[14]	Hong Y Y, Liu Y M, Chen X Y, et al. The role of anthropogenic chlorine emission in surface ozone formation during different seasons over eastern China [J]. Science of the Total Environment, 2020,723: 137697.
[15]	Li L, Yin S J, Huang L, et al. An emission inventory for Cl2 and HOCl in Shanghai, 2017 [J]. Atmospheric Environment, 2020,223:117220.
[16]	Liu Y M, Fan Q, Chen X Y, et al. Modeling the impact of chlorine emissions from coal combustion and prescribed waste incineration on tropospheric ozone formation in China [J]. Atmospheric Chemistry and Physics, 2018,18(4):2709-2724.
[17]	Qiu X H, Ying Q, Wang S X, et al. Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing, China [J]. Atmospheric Chemistry and Physics, 2019, 19(10):6737-6747.
[18]	Yi X, Yin S J, Huang L, et al. Anthropogenic emissions of atomic chlorine precursors in the Yangtze River Delta region, China [J]. Science of the Total Environment, 2021,771:144644.
[19]	Wang X, Jacob D J, Fu X, et al. Effects of anthropogenic chlorine on PM2.5 and Ozone air quality in China [J]. Environmental Science & Technology, 2020,54(16):9908-9916.
[20]	Zhang Y Z, Liu J F, Tao W, et al. Impacts of chlorine emissions on secondary pollutants in China [J]. Atmospheric Environment, 2021, 246:118177.
[21]	Mcculloch A, Aucott M L, Benkovitz C M, et al. Global emissions of hydrogen chloride and chloromethane from coal combustion, incineration and industrial activities: Reactive Chlorine Emissions Inventory [J]. Journal of Geophysical Research: Atmospheres, 1999, 104(D7):8391-8403.
[22]	Li J Y, Zhang N, Wang P, et al. Impacts of chlorine chemistry and anthropogenic emissions on secondary pollutants in the Yangtze river delta region [J]. Environmental Pollution, 2021,287:117624.
[23]	Byun D, Schere K L. Review of the governing equations, computational algorithms, and other components of the Models- 3Community Multiscale Air Quality (CMAQ) modeling system [J]. Applied Mechanics Reviews, 2006,59(2):51-77.
[24]	Xie Y, Paulot F, Carter W, et al. Understanding the impact of recent advances in isoprene photooxidation on simulations of regional air quality [J]. Atmospheric Chemistry & Physics Discussions, 2012,12: 27173-27218.
[25]	Hutzell W T, Luecken D J, Appel K W, et al. Interpreting predictions from the SAPRC07 mechanism based on regional and continental simulations [J]. Atmospheric Environment, 2012,46:417-429.
[26]	Carter W P L. Development of the SAPRC-07 chemical mechanism [J]. Atmospheric Environment, 2010,44(40):5324-5335.
[27]	Sarwar G, Simon H, Xing J, et al. Importance of tropospheric ClNO2 chemistry across the Northern Hemisphere [J]. Geophysical Research Letters, 2014,41(11):4050-4058.
[28]	Sarwar G, Simon H, Bhave P, et al. Examining the impact of heterogeneous nitryl chloride production on air quality across the United States [J]. Atmospheric Chemistry and Physics, 2012,12(14): 6455-6473.
[29]	Pye H O T, Pouliot G A. Modeling the role of alkanes, polycyclic aromatic hydrocarbons, and their oligomers in secondary organic aerosol formation [J]. Environmental Science & Technology, 2012, 46(11):6041-6047.
[30]	Pye H O T, Pinder R W, Piletic I R, et al. Epoxide pathways improve model predictions of isoprene markers and reveal key role of acidity in aerosol formation [J]. Environmental Science & Technology, 2013, 47(19):11056-11064.
[31]	Pye H O T, Luecken D J, Xu L, et al. Modeling the current and future roles of particulate organic nitrates in the Southeastern United States [J]. Environmental Science & Technology, 2015,49(24):14195-14203.
[32]	Liggio J, Li S M, Mclaren R. Reactive uptake of glyoxal by particulate matter [J]. Journal of Geophysical Research-Atmospheres, 2005, 110(D10):D10304.
[33]	Seisel S, Flückiger B, Caloz F, et al. Heterogeneous reactivity of the nitrate radical: reactions on halogen salt at ambient temperature and on ice in the presence of HX (X=Cl, Br, I) at 190K [J]. Physical Chemistry Chemical Physics, 1999,1(9):2257-2266.
[34]	Guenther A B, Jiang X, Heald C L, et al. The model of emissions of gases and aerosols from Nature version 2.1 (MEGAN2.1): An extended and updated framework for modeling biogenic emissions [J]. Geoscientific Model Development, 2012,5(6):1471-1492.
[35]	Gantt B, Kelly J T, Bash J O. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2 [J]. Geoscientific Model Development, 2015,8(11):3733-3746.
[36]	Li M, Zhang Q, Kurokawa J I, et al. MIX: a mosaic Asian anthropogenic emission inventory under the international collaboration framework of the MICS-Asia and HTAP [J]. Atmospheric Chemistry and Physics, 2017,17(2):935-963.
[37]	Janssens-Maenhout G, Crippa M, Guizzardi D, et al. HTAP_v2.2: a mosaic of regional and global emission grid maps for 2008and 2010to study hemispheric transport of air pollution [J]. Atmospheric Chemistry and Physics, 2015,15(19):11411-11432.
[38]	Pio C A, Harrison R M. Vapour pressure of ammonium chloride aerosol: Effect of temperature and humidity [J]. Atmospheric Environment (1967), 1987,21(12):2711-2715.