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潜在亚硝酸源增强二次污染物的能力不一致:来自WRF-Chem模型的证据。

Inconsistent capacity of potential HONO sources to enhance secondary pollutants: Evidence from WRF-Chem modeling.

作者信息

Zhang Jingwei, Ran Haiyan, Qu Yu, Lian Chaofan, Wang Weigang, Zhang Yusheng, Zheng Feixue, Fan Xiaolong, Lu Dawei, Yan Chao, Daellenbach Kaspar R, Ma Zhiqiang, Liu Yongchun, Ge Maofa, Kulmala Markku, An Junling

机构信息

Yunnan Key Laboratory of Meteorological Disasters and Climate Resources in the Greater Mekong Subregion, Yunnan University, Kunming 650500, China; State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics (IAP), Chinese Academy of Sciences, Beijing 100029, China.

State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics (IAP), Chinese Academy of Sciences, Beijing 100029, China; College of Earth and Planetary Sciences, University of the Chinese Academy of Sciences, Beijing 100049, China.

出版信息

J Environ Sci (China). 2025 Dec;158:812-830. doi: 10.1016/j.jes.2025.02.023. Epub 2025 Feb 22.

Abstract

Nitrous acid (HONO) is a crucial source of OH radicals in the troposphere, significantly enhancing secondary pollutants like secondary organic aerosols (SOA) and peroxyacetyl nitrates (PAN). While prior research has examined HONO sources and their total impacts on secondary pollution, the specific enhancement capacity of each individual HONO source remains underexplored. This study uses observational data from 2015 to 2018 for HONO, SOA, and PAN across six sites in China, combined with WRF-Chem model adding six potential HONO sources to evaluate their capacity: traffic emissions (E_traffic), soil emissions (E_soil), indoor-outdoor exchange (E_indoor), nitrate photolysis (P_nit), and NO heterogeneous reactions on aerosol and ground surfaces (Het_a, Het_g). The simulated HONO contributions near the ground in urban Beijing were: 12 % from NO + OH (default source), 10 %-20 % from E_traffic, 1 %-12 % from P_nit, 2 %-10 % from Het_a, and 50 %-70 % from Het_g. For SOA and PAN, we calculated incremental contributions enhanced by each HONO source and derived enhancement ratios (ERs) normalized against HONO's contribution: ∼7 for P_nit, ∼2 for Het_a, ∼0.9 for Het_g, ∼0.8 for E_soil, ∼0.3 for E_traffic, and ∼0.1 for E_indoor. HONO sources' capacity to enhance secondary pollutants varies, being larger for aerosol-related sources. Vertical analysis on HONO concentration, spatial distribution, RO radical cycling rates, and OH enhancements revealed that aerosol-related HONO sources, especially P_nit, contribute more to secondary pollution. Future research should focus more on assessing real-world impacts of HONO sources, besides identifying their budgets. Additionally, uptake coefficient (γ) and nitrate photolysis frequency (J) critically affect HONO and secondary pollutant formation, necessitating further investigations.

摘要

亚硝酸(HONO)是对流层中羟基自由基的重要来源,能显著增加二次有机气溶胶(SOA)和过氧乙酰硝酸酯(PAN)等二次污染物。虽然先前的研究已经考察了HONO的来源及其对二次污染的总体影响,但各个HONO来源的具体增强能力仍未得到充分探索。本研究利用2015年至2018年中国六个站点的HONO、SOA和PAN观测数据,结合添加了六种潜在HONO来源的WRF-Chem模型来评估它们的能力:交通排放(E_traffic)、土壤排放(E_soil)、室内外交换(E_indoor)、硝酸盐光解(P_nit)以及气溶胶和地面表面的NO非均相反应(Het_a、Het_g)。在北京城区地面附近模拟的HONO贡献为:NO + OH(默认来源)占12%,E_traffic占10% - 20%,P_nit占1% - 12%,Het_a占2% - 10%,Het_g占50% - 70%。对于SOA和PAN,我们计算了每个HONO来源增强的增量贡献,并得出相对于HONO贡献进行归一化的增强率(ERs):P_nit约为7,Het_a约为2,Het_g约为0.9,E_soil约为0.8,E_traffic约为0.3,E_indoor约为0.1。HONO来源增强二次污染物的能力各不相同,与气溶胶相关的来源增强能力更大。对HONO浓度、空间分布、RO自由基循环速率和OH增强的垂直分析表明,与气溶胶相关的HONO来源,尤其是P_nit,对二次污染的贡献更大。未来的研究除了确定HONO来源的收支情况外,应更多地关注评估其在现实世界中的影响。此外,摄取系数(γ)和硝酸盐光解频率(J)对HONO和二次污染物的形成至关重要,需要进一步研究。

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