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秋季北京大气氧化能力:基于观测模型的 O 和 PM 事件分析。

Atmospheric oxidizing capacity in autumn Beijing: Analysis of the O and PM episodes based on observation-based model.

机构信息

State Key Laboratory for Structural Chemistry of Unstable and Stable Species, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

State Key Laboratory for Structural Chemistry of Unstable and Stable Species, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

出版信息

J Environ Sci (China). 2023 Feb;124:557-569. doi: 10.1016/j.jes.2021.11.020. Epub 2022 Feb 23.

Abstract

Atmospheric oxidizing capacity (AOC) is the fundamental driving factors of chemistry process (e.g., the formation of ozone (O) and secondary organic aerosols (SOA)) in the troposphere. However, accurate quantification of AOC still remains uncertainty. In this study, a comprehensive field campaign was conducted during autumn 2019 in downtown of Beijing, where O and PM episodes had been experienced successively. The observation-based model (OBM) is used to quantify the AOC at O and PM episodes. The strong intensity of AOC is found at O and PM episodes, and hydroxyl radical (OH) is the dominating daytime oxidant for both episodes. The photolysis of O is main source of OH at O episode; the photolysis of nitrous acid (HONO) and formaldehyde (HCHO) plays important role in OH formation at PM episode. The radicals loss routines vary according to precursor pollutants, resulting in different types of air pollution. O budgets and sensitivity analysis indicates that O production is transition regime (both VOC and NO-limited) at O episode. The heterogeneous reaction of hydroperoxy radicals (HO) on aerosol surfaces has significant influence on OH and O production rates. The HO uptake coefficient (γHO) is the determining factor and required accurate measurement in real atmospheric environment. Our findings could provide the important bases for coordinated control of PM and O pollution.

摘要

大气氧化性(AOC)是对流层化学过程(例如臭氧(O)和二次有机气溶胶(SOA)的形成)的基本驱动力。然而,AOC 的准确量化仍然存在不确定性。在本研究中,于 2019 年秋季在北京市中心进行了一次全面的野外考察,期间相继经历了 O 和 PM 事件。使用基于观测的模型(OBM)来量化 O 和 PM 事件期间的 AOC。在 O 和 PM 事件期间,发现 AOC 的强度很强,并且 OH 是两个事件的主要日间氧化剂。O 的光解是 O 事件中 OH 的主要来源;在 PM 事件中,HONO 和 HCHO 的光解在 OH 形成中起重要作用。根据前体污染物的不同,自由基损耗过程也不同,导致不同类型的空气污染。O 预算和敏感性分析表明,在 O 事件中,O 的生成处于过渡状态(VOC 和 NO 均受限)。HO 在气溶胶表面上的非均相反应对 OH 和 O 的生成速率有显著影响。HO 吸收系数(γHO)是决定因素,在实际大气环境中需要准确测量。我们的研究结果可为 PM 和 O 污染的协同控制提供重要依据。

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