State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China; College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China; College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
J Environ Sci (China). 2023 Jan;123:350-366. doi: 10.1016/j.jes.2022.06.029. Epub 2022 Jul 1.
Atmospheric oxidizing capacity (AOC) is an essential driving force of troposphere chemistry and self-cleaning, but the definition of AOC and its quantitative representation remain uncertain. Driven by national demand for air pollution control in recent years, Chinese scholars have carried out studies on theories of atmospheric chemistry and have made considerable progress in AOC research. This paper will give a brief review of these developments. First, AOC indexes were established that represent apparent atmospheric oxidizing ability (AOIe) and potential atmospheric oxidizing ability (AOIp) based on aspects of macrothermodynamics and microdynamics, respectively. A closed study refined the quantitative contributions of heterogeneous chemistry to AOC in Beijing, and these AOC methods were further applied in Beijing-Tianjin-Hebei and key areas across the country. In addition, the detection of ground or vertical profiles for atmospheric OH·, HO·, NO· radicals and reservoir molecules can now be obtained with domestic instruments in diverse environments. Moreover, laboratory smoke chamber simulations revealed heterogeneous processes involving reactions of O and NO, which are typical oxidants in the surface/interface atmosphere, and the evolutionary and budgetary implications of atmospheric oxidants reacting under multispecies, multiphase and multi-interface conditions were obtained. Finally, based on the GRAPES-CUACE adjoint model improved by Chinese scholars, simulations of key substances affecting atmospheric oxidation and secondary organic and inorganic aerosol formation have been optimized. Normalized numerical simulations of AOIe and AOIp were performed, and regional coordination of AOC was adjusted. An optimized plan for controlling O and PM was analyzed by scenario simulation.
大气氧化性(AOC)是对流层化学和自净的重要驱动力,但 AOC 的定义及其定量表示仍不确定。近年来,受国家对空气污染控制的需求驱动,中国学者开展了大气化学理论研究,并在 AOC 研究方面取得了相当大的进展。本文将简要回顾这些进展。首先,建立了 AOC 指标,分别基于宏观热力学和微观动力学,代表明显的大气氧化能力(AOIe)和潜在的大气氧化能力(AOIp)。一个封闭的研究细化了异质化学对北京 AOC 的定量贡献,这些 AOC 方法进一步应用于京津冀和全国重点地区。此外,现在可以使用国内仪器在各种环境中检测大气 OH·、HO·、NO·自由基和储库分子的地面或垂直分布。此外,实验室烟雾室模拟揭示了涉及表面/界面大气中典型氧化剂 O 和 NO 反应的非均相过程,获得了大气氧化剂在多物种、多相和多界面条件下反应的演化和预算影响。最后,基于中国学者改进的 GRAPES-CUACE 伴随模型,对影响大气氧化和二次有机及无机气溶胶形成的关键物质的模拟进行了优化。对 AOIe 和 AOIp 进行了归一化数值模拟,并对 AOC 进行了区域协调调整。通过情景模拟分析了优化的 O 和 PM 控制方案。