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在氮氧化物浓度降低的情况下,将臭氧增加归因于挥发性有机化合物的加速氧化。

Attributing Increases in Ozone to Accelerated Oxidation of Volatile Organic Compounds at Reduced Nitrogen Oxides Concentrations.

作者信息

Zhang Zekun, Jiang Jiakui, Lu Bingqing, Meng Xue, Herrmann Hartmut, Chen Jianmin, Li Xiang

机构信息

Department of Environmental Science & Engineering, Fudan University, Shanghai 200032, China.

Leibniz-Institut für Troposphärenforschung (IfT), Permoserstr. 15, 04318 Leipzig, Germany.

出版信息

PNAS Nexus. 2022 Nov 18;1(5):pgac266. doi: 10.1093/pnasnexus/pgac266. eCollection 2022 Nov.

Abstract

Surface ozone (O) is an important secondary pollutant affecting climate change and air quality in the atmosphere. Observations during the COVID-19 lockdown in urban China show that the co-abatement of nitrogen oxides (NO) and volatile organic compounds (VOCs) caused winter ground-level O increases, but the chemical mechanisms involved are unclear. Here we report field observations in the Shanghai lockdown that reveals increasing photochemical formation of O from VOC oxidation with decreasing NO. Analyses of the VOC profiles and NO/NO indicate that the O increases by the NO reduction counteracted the O decreases through the VOC emission reduction in the VOC-limited region, and this may have been the main mechanism for this net O increase. The mechanism may have involved accelerated OH-HO-RO radical cycling. The NO reductions for increasing O production could explain why O increased from 2014 to 2020 in response to NO emission reduction even as VOC emissions have essentially remained unchanged. Model simulations suggest that aggressive VOC abatement, particularly for alkenes and aromatics, should help reverse the long-term O increase under current NO abatement conditions.

摘要

地表臭氧(O)是一种重要的二次污染物,会影响大气中的气候变化和空气质量。在中国城市新冠疫情封锁期间的观测表明,氮氧化物(NO)和挥发性有机化合物(VOCs)的协同减排导致冬季地面臭氧增加,但其涉及的化学机制尚不清楚。在此,我们报告了上海封锁期间的实地观测结果,结果显示随着NO的减少,VOC氧化产生的臭氧光化学生成增加。对VOCs剖面和NO/NO的分析表明,在VOCs受限区域,NO减少导致的臭氧增加抵消了VOCs排放减少导致的臭氧减少,这可能是臭氧净增加的主要机制。该机制可能涉及加速的OH-HO-RO自由基循环。为增加臭氧生成而进行的NO减排可以解释为什么即使VOCs排放基本保持不变,臭氧在2014年至2020年期间仍因NO排放减少而增加。模型模拟表明,积极减少VOCs排放,特别是减少烯烃和芳烃的排放,应有助于在当前NO减排条件下扭转臭氧长期增加的趋势。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/765a/9802302/b5cc9e1a450a/pgac266fig1.jpg

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