区域大气环境模式RegAEMS中二次气溶胶的改进模拟研究

摘要
图/表
参考文献
相关文章 (15)

全文: PDF (1921 KB) HTML (0 KB)
输出: BibTeX | EndNote (RIS)

摘要为了提升二次气溶胶的模拟精度，在区域大气环境模式RegAEMS中加入了硫酸盐气溶胶的两种新生成机制（NO₂+SO₂化学过程和过渡金属催化氧化（TMI））以及二次有机气溶胶（SOA）生成的挥发性有机物基集（VBS）方法.模拟了2020年1月上海市两次中度污染过程，并与观测数据进行对比验证.研究发现，两次污染过程硫氧转化率（SOR）均大于0.4，PM_2.5主要组分为SO₄^2-、NO₃^-、NH₄⁺等水溶性离子，占比为61.25%~63.85%.SOA占比为2.92%~3.0%.加入NO₂+SO₂化学过程和过渡金属催化氧化（TMI）后，硫酸盐模拟精度明显提升（相关系数（R）从0.49~0.63提升至0.58~0.67，相对标准偏差（NMB）从-35.0%~-36.5%提升至-17.3%~-14.2%）.两种化学过程在污染发展阶段平均贡献占比为23.3%~27.9%，这可能是造成污染条件下SO₄^2-浓度迅速增加的主要原因.VBS机制能够较好地模拟出SOA的变化趋势（相关系数为0.53~0.56），由于硫酸盐和SOA生成机理的改进，RegAEMS在PM_2.5的模拟精度上有所提升（相对标准偏差（NMB）从-13.5%~-6.0%提升至-9.0%~-3.3%）.

	服务

	把本文推荐给朋友
	加入我的书架
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	罗干
	王体健
	李蒙蒙
	徐北瑶
	谢旻
	李树
	伏晴艳

关键词 ： PM_2.5, 硫酸盐, VBS, RegAEMS, 数值模拟

Abstract：In order to improve the accuracy of the secondary aerosol simulation, this study added two new formation mechanisms of sulfate (NO₂+SO₂ chemical process and heterogeneous transition-metal-catalyzed oxidation (TMI)) and volatile organic compounds (VBS) based on the regional atmospheric environment model RegAEMS. The two moderate pollution processes in shanghai in January 2020 were simulated and compared with observational data for verification. The study found that the sulfur oxygen conversion rate(SOR) of the two pollution processes were both greater than 0.4, and the main components of PM_2.5 were sulfate, nitrate and ammonium, accounting for 61.25% to 63.85%. SOA accounted for 2.92%~3.0%. After the addition of the NO₂+SO₂ chemical process and TMI catalytic oxidation, the accuracy of sulfate simulation is significantly improved (The correlation coefficient (R) increased from 0.49~0.63 to 0.58~0.67, and the relative standard deviation (NMB) increased from -35.0%~-36.5% to -17.3%~-14.2%). The average contribution of the two chemical processes during the pollution occurrence stage is 23.3%~27.9%, which may be the main reason for the sudden increase of sulfate^- concentration under pollution conditions. The VBS mechanism can better simulate the change trend of SOA (The correlation coefficient is 0.53~0.56), and the improved model slightly improves the simulation accuracy of PM_2.5 (Relative standard deviation (NMB) increased from -13.5%~-6.0% to -9.0%~-3.3%).

Key words： PM_2.5 sulfate VBS RegAEMS numerical simulation

收稿日期: 2021-03-12

PACS:

X51

基金资助:国家重点研发计划项目（2020YFA0607802，2018YFC0213503）

通讯作者: 王体健,教授,tjwang@nju.edu.cn E-mail: tjwang@nju.edu.cn

作者简介: 罗干(1997-),男,陕西安康人,南京大学硕士研究生,主要研究方向为大气细颗粒物来源解析与数值模拟.

引用本文:

罗干, 王体健, 李蒙蒙, 徐北瑶, 谢旻, 李树, 伏晴艳. 区域大气环境模式RegAEMS中二次气溶胶的改进模拟研究[J]. 中国环境科学, 2021, 41(10): 4541-4548. LUO Gan, WANG Ti-jian, LI Meng-meng, XU Bei-yao, XIE Min, LI Shu, FU Qing-yan. Improved simulation of secondary aerosol in the regional atmospheric environment modeling system RegAEMS. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(10): 4541-4548.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2021/V41/I10/4541

[1]	Zhai S, Jacob D J, Wang X, et al. Fine particulate matter trends in China, 2013-2018:separating contributions from anthropogenic emissions and meteorology[J]. Atmospheric Chemistry and Physics, 2019,19(16):11031-11041.
[2]	张小曳,徐祥德,丁一汇,等.2013~2017年气象条件变化对中国重点地区PM2.5质量浓度下降的影响[J]. 中国科学:地球科学, 2020, 50(4):483-500.Zhang X, Xu X, Ding Y, et al. The impact of meteorological changes from 2013 to 2017 on PM2.5 mass reduction in key regions in China[J]. Science China Earth Sciences, 2019,62:1885-1902.
[3]	Ma Z, Liu R, Liu Y, et al. Effects of air pollution control policies on PM2.5 pollution improvement in China from 2005 to 2017:a satellite-based perspective[J]. Atmos. Chem. Phys., 2019,19:6861-6877.
[4]	Jiang Z, Jolleys M D, Fu T-M, et al. Spatiotemporal and probability variations of surface PM2.5 over China between 2013 and 2019 and the associated changes in health risks:An integrative observation and model analysis[J]. Science of The Total Environment, 2020,723:137896.
[5]	张莹袁,王式功,贾旭伟,等.气温与PM2.5协同作用对疾病急诊就诊人数的影响[J]. 中国环境科学, 2017,37(8):3175-3182.Zhang Y Y, Wang S G, Jia X W, et al. Synergetic effect of mean temperature and PM2.5 on emergency room visits for different diseases[J]. China Environmental Science, 2017,37(8):3175-3182.
[6]	Matus K, Nam K-M, Selin N E, et al. Health damages from air pollution in China[J]. Global Environmental Change, Global Environmental Change, 2012,22(1):55-66.
[7]	Pui D Y H, Chen S-C, Zuo Z, et al. PM2.5 in China:Measurements, sources, visibility and health effects, and mitigation[J]. Particuology, Particuology, 2014,13:1-26.
[8]	Guo S, Hu M, Zamora M L, et al. Elucidating severe Urban haze formation in China[J]. Proceeding of the National Academy of Science, 2014,111(49):17373-17378.
[9]	He K, Huo H, Zhang Q, et al. Urban air pollution in China:Current status, characteristics, and progress[J]. Annual Review of Energy and the Environment, Annual Review of Energy and the Environment, 2002,27(1):397-431.
[10]	Wang G, Zhang R, Gomez M E, et al. Persistent sulfate formation from London Fog to Chinese haze[J]. Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, 2016,113(48):13630-13635.
[11]	Cheng Y, Zheng G, Wei C, et al. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China[J]. Science Advances, Science Advances, 2016,2(12):e1601530.
[12]	Guo H, Weber R J, Nenes A, et al. High levels of ammonia do not raise fine particle pH sufficiently to yield nitrogen oxide-dominated sulfate production[J]. Scientific Reports, Scientific Reports, 2017,7(1).
[13]	Yue F, He P, Chi X, et al. Characteristics and major influencing factors of sulfate production via heterogeneous transition-metal-catalyzed oxidation during haze evolution in China[J]. Atmospheric Pollution Research, Atmospheric Pollution Research, 2020,11(8):1351-1358.
[14]	Huang L, An J, Koo B, et al. Sulfate formation during heavy winter haze events and the potential contribution from heterogeneous SO2+ NO2 reactions in the Yangtze River Delta region, China[J]. Atmospheric Chemistry and Physics, Atmospheric Chemistry and Physics, 2019,19(22):14311-14328.
[15]	Jiang F, Liu Q, Huang X, et al. Regional modeling of secondary organic aerosol over China using WRF/Chem[J]. Journal of Aerosol Science, Journal of Aerosol Science, 2012,43(1):57-73.
[16]	Chen X, Yang W, Wang Z, et al. Improving new particle formation simulation by coupling a volatility-basis set (VBS) organic aerosol module in NAQPMS+APM[J]. Atmospheric Environment, Atmospheric Environment, 2019,204:1-11.
[17]	Woody M C, Baker K R, Hayes P L, et al. Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS[J]. Atmospheric Chemistry and Physics, Atmospheric Chemistry and Physics, 2016,16(6):4081-4100.
[18]	Ahmadov R, Mckeen S A, Robinson A L, et al. A volatility basis set model for summertime secondary organic aerosols over the eastern United States in 2006[J]. Journal of Geophysical Research:Atmospheres, Journal of Geophysical Research:Atmospheres, 2012, 117(D06301).
[19]	朱佳雷,王体健,邓君俊,等.长三角地区秸秆焚烧污染物排放清单及其在重霾污染天气模拟中的应用[J]. 环境科学学报, 2012,32(12):3045-3055.Zhu J L, Wang T J, Deng J J, et al. An emission inventory of air pollutants from crop residue burning Yangtze River Delta region and its application in simulation of a heavy haze weather process[J]. Acta Sci Circumst, 2012,32:3045-3055.
[20]	陈璞珑,王体健,谢晓栋,等.基于数值模式的细颗粒物来源解析[J]. 科学通报, 2018,63(18):1829-1838.Chen P L, Wang T J, Xie X D, et al. Source apportionment of fine particles based on combined numerical model and receptor model (in Chinese)[J]. Chinese Science Bulletin, 2018,63(18):1829-1838.
[21]	Zhang Q, Streets D G, Carmichael G R, et al. Asian emissions in 2006 for the NASA INTEX-B mission. Atmos Environ, 2009,9:5131-5153.
[22]	J. H. Seinfeld, S. N. Pandis, Atmospheric Chemistry and Physics, from Air Pollution to Climate Change (Wiley, 2006)[M].
[23]	Fountoukis C, Nenes A. ISORROPIA II:a computationally efficient thermodynamic equilibrium model for K+-Ca2+-Mg2+-NH4+-Na+-SO42-[J]. Atmospheric Chemistry and Physics, Atmospheric Chemistry and Physics, 2007,7(17):4639-4659.
[24]	He P, Alexander B, Geng L, et al. Isotopic constraints on heterogeneous sulfate production in Beijing haze[J]. Atmospheric Chemistry and Physics, Atmospheric Chemistry and Physics, 2018, 18(8):5515-5528.
[25]	Takashi Ibusuki, Koji Takeuchi. Sulfur dioxide oxidation by oxygen catalyzed by mixtures of manganese(II) and iron(III) in aqueous solutions at environmental reaction conditions[J]. Atmospheric Environment, 1967,21(7):1555-1560.
[26]	Donahue N M, Epstein S A, Pandis S N, et al. A two-dimensional volatility basis set:1. organic-aerosol mixing thermodynamics[J]. Atmospheric Chemistry and Physics, Atmospheric Chemistry and Physics, 2011,11(7):3303-3318.
[27]	Lin J, An J, Qu Y, et al. Local and distant source contributions to secondary organic aerosol in the Beijing urban area in summer[J]. Atmospheric Environment, Atmospheric Environment, 2016,124:176-185.
[28]	Shrivastava M K, Lane T E, Donahue N M, et al. Effects of gas particle partitioning and aging of primary emissions on urban and regional organic aerosol concentrations[J]. Journal of Geophysical Research:Atmospheres, Journal of Geophysical Research:Atmospheres, 2008,113(D18).
[29]	黄炯丽,陈志明,莫招育,等.基于高分辨率MARGA分析桂林市PM2.5水溶性离子特征[J]. 中国环境科学, 2019,39(4):1390-1404.Huang J L, Chen Z M, Mo Z Y, et al. Analysis of characteristics of water-soluble ions in PM2.5 in Guilin based on the MARGA[J]. China Environmental Science, 2019,39(4):1390-1404.
[30]	Yao X H, Chan C K, Fang M, et al. The water-soluble ionic composition of PM2.5 in Shanghai and Beijing, China[J]. Atmospheric Environment, 2002,36(26):4223-4234.
[31]	叶文媛,吴彬,冯银厂,等.大气中二次有机气溶胶估算方法研究进展[J]. 安全与环境学, 2011,11(1):127-131.Ye W Y, Wu B, Feng Y C, et al. Advances in the estimation methods of secondary organic aerosol in atmospheric environment[J]. Journal of safety and Environment, 2011,11(1):127-131.