ISSN 1008-5548

CN 37-1316/TU

最新出版

中国大气二次有机气溶胶产率、化学机制与模型参数化研究进展

Research progress on yields, chemical mechanisms, and model parameterization of atmospheric secondary organic aerosol in China


臧寒1, 周琪琦2, 赵岳1, 郭松2

1.上海交通大学 环境科学与工程学院, 上海 200240; 2.北京大学 区域环境安全全国重点实验室 环境科学与工程学院, 北京 100871

引用格式:

臧寒, 周琪琦, 赵岳, 等. 中国大气二次有机气溶胶产率、化学机制与模型参数化研究进展[J]. 中国粉体技术, 2027, 33(2): 1-14.

Zang Han, Zhou Qiqi, Zhao Yue, et al. Research progress on yields, chemical mechanisms, and model parameterization of atmospheric secondary organic aerosol in China [J]. China Powder Science and Technology, 2027, 33(2): 1-14.

DOI:10.13732/j.issn.1008-5548.2027.02.015

收稿日期: 2026-08-06, 修回日期: 2026-09-16, 上线日期: 2026-10-09。

基金项目: 国家自然科学基金项目,编号:22376137; 国家重点研发计划项目,编号:2022YFC3701003。

第一作者: 臧寒(1994—),女,博士后,博士,研究方向为大气二次有机气溶胶生成机制。E-mail:zanghan@sjtu.edu.cn。

通信作者: 赵岳(1986—),男,教授,博士,博士生导师,国家自然科学基金优秀青年科学基金获得者,研究方向为大气活性有机物化学行为及效应。E-mail:yuezhao20@sjtu.edu.cn。郭松(1982—),男,研究员,博士,博士生导师,海外高层次人才(青年),环保部青年拔尖人才,研究方向为大气环境化学。E-mail:songguo@pku.edu.cn。

摘要: 【目的】 为了厘清我国大气二次有机气溶胶(secondary organic aerosol, SOA)生成机制研究的发展脉络与研究现状,明晰当前SOA化学机制的认知水平、关键问题与核心瓶颈,并明确未来重点方向,从而实现我国大气复合污染条件下细颗粒物的精准防控。 【研究现状】 系统总结我国大气复合污染条件下SOA的生成特征,综述国内学者在SOA生成产率,气相、液相、非均相生成机制,参数化及模型模拟方面的研究进展;在此基础上,梳理我国SOA机制研究 “由简化至复合体系”“由定性解释至定量约束”的演进历程及代表性成果;概述SOA模型模拟由固定产率和双产物方案,向综合表征有机物挥发性、气粒分配、多代氧化以及液相和非均相反应的参数化框架的发展过程,指出当前核心瓶颈集中于SOA产率环境依赖性缺乏系统性定量认识、关键化学机制尚不明晰、相关过程参数化方案严重缺失。 【结论与展望】 提出未来亟须拓宽前体物边界、突破多前体物多氧化剂协同机制及气-液-非均相过程耦合机制、发展适用于我国大气复合污染条件的SOA生成参数化方案,以深化对典型城市群与背景区域SOA来源贡献及生成机制的理解,为细颗粒物与臭氧污染协同控制提供更坚实的科学支撑。

关键词: 二次有机气溶胶; 挥发性有机物; 气相氧化; 液相反应; 非均相反应; 产率; 模型模拟

Abstract 

Significance Secondary organic aerosol (SOA), a major component of atmospheric fine particulate matter (PM2.5), has substantial effects on air quality, climate, and public health. It is formed through the atmospheric oxidation of reactive organic carbon, including volatile organic compounds (VOCs), intermediate-volatility organic compounds (IVOCs), and semi-volatile organic compounds (SVOCs), followed by gas–particle partitioning and aqueous-phase, interfacial, and heterogeneous transformations. The diversity of precursors, continuous evolution of product volatility and reactivity, and coupling of multiple chemical processes make SOA formation a persistent challenge for atmospheric observation and modeling. This challenge is particularly prominent in China, where intensive anthropogenic emissions, biogenic precursors, high concentrations of inorganic pollutants, multiple oxidants, and abundant aerosol liquid water coexist. Since 2013, substantial reductions in sulfur dioxide, nitrogen oxides, and primary particulate matter emissions have led to decreases in PM2.5 and organic aerosol concentrations, whereas the relative contribution of SOA to organic aerosol has increased. Understanding SOA formation is therefore increasingly important for further air quality improvement and the coordinated control of PM2.5 and ozone.

Progress This review systematically summarizes the formation characteristics of SOA under complex atmospheric pollution conditions in China, as well as research conducted by Chinese scholars on SOA yields, gas-phase oxidation, aqueous-phase and heterogeneous chemistry, parameterization, and regional modeling. SOA yield studies have evolved from measurements of individual VOCs in simplified oxidation systems to investigations of mixed precursors and complex emissions from vehicles, biomass burning, and cooking sources. These studies demonstrate that SOA yields depend strongly on nitrogen oxides, seed aerosol composition, organic aerosol loading, temperature, relative humidity, coexisting oxidants, and radical chemistry. IVOCs and SVOCs have consequently emerged as important previously missing precursors in conventional emission inventories. Gas-phase mechanism research has progressed from product identification to molecular-level characterization of organic peroxy radical (RO2) chemistry, autoxidation, highly oxygenated organic molecule formation, and the competing effects of functionalization and fragmentation. The nonlinear influence of nitrogen oxides and interactions among RO2 radicals from different precursors explain why SOA formation in mixed systems may be either enhanced or suppressed relative to linear predictions. Research on aqueous-phase and heterogeneous chemistry has similarly advanced from reactions of small oxygenated compounds on mineral particles or in dilute solutions to reactive uptake, photochemistry, and organic peroxide transformations in atmospherically relevant aerosol particles and microdroplets. Modeling approaches have developed from fixed-yield and two-product schemes to volatility basis set (VBS) and two-dimensional volatility basis set (2D-VBS) frameworks that represent primary organic aerosol evaporation, IVOC oxidation, multigenerational aging, volatility evolution, and aerosol oxidation state. China-specific emission inventories and improved reactive uptake schemes have enhanced model performance, but substantial model-observation discrepancies remain because environmental dependencies, multiphase kinetics, and several key reaction pathways are still inadequately constrained.

Conclusions and Prospects Looking forward, this review proposes that future efforts should prioritize broadening the range of precursor species, advancing the understanding of synergistic mechanisms in multi-precursor and multi-oxidant systems, improving the understanding of coupled gas-phase, aqueous-phase, and heterogeneous processes, and developing SOA formation parameterization schemes tailored to China’s complex atmospheric pollution conditions. These advances are essential for deepening the understanding of SOA source contributions and formation pathways in typical urban clusters and background regions, thereby providing a more robust scientific basis for the synergistic control of PM2.5 and ozone pollution in China.

Keywords: secondary organic aerosol; volatile organic compound; gas-phase oxidation; aqueous-phase reaction; heterogeneous reaction; formation yield; model simulation

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