ISSN 1008-5548

CN 37-1316/TU

最新出版

中国大气二次有机气溶胶定量估算与前体物基础研究进展

Research progress on quantitative estimation and precursor basis of atmospheric secondary organic aerosols in China


周琪琦1, 臧寒2, 赵岳2, 郭松1

1.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;2.上海交通大学 环境科学与工程学院, 上海 200240


引用格式:

周琪琦, 臧寒, 赵岳, 等. 中国大气二次有机气溶胶定量估算与前体物基础研究进展[J]. 中国粉体技术, 2027, 33(2): 1-15.

Zhou Qiqi, Zang Han, Zhao Yue, et al. Research progress on quantitative estimation and precursor basis of atmospheric secondary organic aerosols in China[J]. China Powder Science and Technology, 2027, 33(2): 1-15.

DOI:10.13732/j.issn.1008-5548.2027.02.010

收稿日期:2026-08-04,修回日期:2026-09-10,上线日期:2026-09-17。

基金项目:国家重点研发项目,编号:2022YFC3701002;区域环境安全全国重点实验室专项经费,编号:26Y01RESPKU。

第一作者:周琪琦(2003—),男,博士研究生,研究方向为大气环境化学。E-mail:zhouqiqichem@stu.pku.edu.cn。

通信作者:郭松(1982—),男,研究员,博士,博士生导师,海外高层次人才引进计划(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;

通信作者:赵岳(1986—),男,教授,博士,博士生导师,国家优青,研究方向为大气二次有机气溶胶生成与演化机制。E-mail:yuezhao20@sjtu.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)定量估算与前体物基础的发展脉络,开展观测识别、源谱测量和排放表征研究进展的系统梳理,为实现源排放至环境SOA的质量闭合提供依据。【研究现状】综述碳质示踪、水溶性有机碳、分子标志物、在线气溶胶质谱及前体物光化学损耗等SOA定量估算方法及其适用边界;概括SOA前体物由传统挥发性有机物向中等挥发性、半挥发性和含氧有机物及未解析复杂混合物拓展的过程;总结我国本土源谱、外场识别与全挥发性排放清单的代表性进展,部分地区的观测结果表明,元素碳示踪法估算的二次有机碳浓度相比正定矩阵因子分解法估算的结果高4%~212%,纳入中等和半挥发性有机物后,模型对观测SOA浓度的解释比例由18%提高至40%。【结论与展望】提出颗粒相定量、气态前体物损耗、源排放谱和模型清单的多证据联合约束路径;认为未来须统一不同SOA观测量的转换边界,完善全挥发性反应性有机碳源谱与动态清单,加强源测试生成潜势和真实环境贡献的交叉验证,为细颗粒物与臭氧协同控制提供科学支撑。

关键词:二次有机气溶胶;前体物源谱;中等挥发性有机物;半挥发性有机物;反应性有机碳;全挥发性排放清单

Abstract

Significance Secondary organic aerosol (SOA) is an important component of atmospheric organic aerosol and contributes substantially to fine-particle pollution, visibility degradation, climate effects, and human health risks. Quantifying ambient SOA and identifying the gaseous precursors and emission sources that sustain its formation are two fundamental and closely connected challenges. These challenges are particularly important in China, where intensive emissions from transportation, industry, coal combustion, solvent use, cooking, biomass burning, and biogenic sources interact under high nitrogen oxide levels, strong atmospheric oxidizing capacity, high aerosol liquid water content, and regional transport. To clarify the development of SOA quantification and precursor characterization in China, advances in observational identification, source profile measurement, ambient precursor detection, and emission inventories are reviewed, with emphasis on contributions from Chinese researchers and mass closure from source emissions to ambient SOA.

Progress SOA quantification in China has evolved from operational estimates based on organic carbon-to-elemental carbon ratios and the elemental carbon tracer method to multiple-evidence constraints using water-soluble organic carbon, chemical mass balance with molecular markers, molecular tracer yield methods, online aerosol mass spectrometry coupled with positive matrix factorization or multilinear engine 2, and volatile organic compound photochemical loss-yield approaches. Early measurements of carbonaceous aerosols established the widespread occurrence of secondary organic carbon in Chinese cities and regional background areas. Subsequent molecular and online measurements improved chemical specificity, temporal resolution, and source interpretation, revealing that oxygenated organic aerosol is commonly an important component during regional transport and atmospheric aging. Comparisons among methods demonstrate that their target quantities and mass boundaries are not equivalent. Secondary organic carbon estimated with the elemental carbon tracer method can be 4%-212% higher than that derived from positive matrix factorization because primary organic carbon-to-elemental carbon ratios vary among emission sources and atmospheric processes. Molecular tracer yield methods may explain only part of total secondary organic carbon, whereas oxygenated organic aerosol cannot be assigned uniquely to a specific precursor or emission source. These findings shift the emphasis from seeking a single optimal estimate to establishing comparable mass bases, uncertainty ranges, and complementary observational constraints.

Conclusions and Prospects A multiple-evidence framework integrating particle-phase quantification, gas-phase precursor loss,locally measured source profiles, ambient validation, and full-volatility emission inventories is required to improve SOA mass closure in China. Future studies should harmonize the definitions and conversion boundaries of secondary organic carbon, SOA, water-soluble organic carbon, and oxygenated organic aerosol; establish standardized full-volatility reactive organic carbon profiles and dynamic emission factors for representative Chinese sources; improve measurements of oxygenated IVOCs, SVOCs, and unresolved mixtures; and strengthen cross-validation among source-test formation potential, ambient precursor loss, particle-phase products, and chemical transport models. These advances will support the coordinated control of fine particulate matter and ozone during deeper emission reductions.

Keywords: secondary organic aerosol; precursor source profile; intermediate-volatility organic compounds; semi-volatile organic compounds; reactive organic carbon; full-volatility emission inventory


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