Gao Zhaoqi, Li Lin, Liu Zhou, Mu Jiangshan, Wang Zhuyi, Luo Bin, Zhang Jingzhu, Tang Shuting, Zhang Hongliang, Hu Jianlin, Wang Xuan, Zhou Xuehua, Zhang Yuqiang
Environment Research Institute, Shandong University, Qingdao, 266237, China.
Environment Research Institute, Shandong University, Qingdao, 266237, China; Department of Environmental Science and Engineering, Fudan University, Shanghai, 200438, China.
Environ Pollut. 2025 Sep 15;381:126524. doi: 10.1016/j.envpol.2025.126524. Epub 2025 May 29.
Chlorine radicals (Cl), as important oxidant in the atmosphere, significantly influence the formation of secondary organic aerosols (SOA), which is harmful to air quality and human health. Additionally, marine is an important source of reactive chlorine-containing species that are released into the atmosphere via sea spray aerosols (SSA). To date, the contribution of marine chlorine-containing species on SOA has not been well quantified. Here, we explored and quantified the impact of chlorine-containing species released by SSA on atmospheric oxidants (Cl, OH, HO, O), SOA and its main components in the North China Plain (NCP) in 2016 based on a high-resolution chemical transport model (WRF-CMAQ). Model results showed that marine chlorine-containing species emissions have the greatest effect on atmospheric oxidants in summer, and can increase Cl up to 4.53 × 10 ppt, reduce OH, HO, and O up to 0.01 ppb, 0.41 ppb, and 5.30 ppb, respectively. Notably, marine chlorine-containing species emissions decreased O generation in each season (up to 1.02 ppb, 3.22 ppb, 5.30 ppb, and 1.58 ppb in winter, spring, summer and autumn, respectively), while promoted SOA formation in winter (0.01 μg/m) and inhibited in summer (0.01 μg/m). We also revealed that under high pollution events in winter, marine chlorine-containing species emissions can increase the SOA formation by up to 0.11 μg/m due to ClNO chemistry (heterogeneous reactions). Our study provides new perspective on the SSA contributions of SOA formation in NCP region.
氯自由基（Cl）作为大气中的重要氧化剂，对二次有机气溶胶（SOA）的形成有显著影响，而SOA对空气质量和人类健康有害。此外，海洋是通过海浪花气溶胶（SSA）释放到大气中的含活性氯物种的重要来源。迄今为止，海洋含氯物种对SOA的贡献尚未得到很好的量化。在此，我们基于高分辨率化学传输模型（WRF-CMAQ），探讨并量化了2016年华北平原（NCP）地区SSA释放的含氯物种对大气氧化剂（Cl、OH、HO₂、O₃）、SOA及其主要成分的影响。模型结果表明，海洋含氯物种排放对夏季大气氧化剂的影响最大，可使Cl增加高达4.53×10⁹ ppt，使OH、HO₂和O₃分别减少高达0.01 ppb、0.41 ppb和5.30 ppb。值得注意的是，海洋含氯物种排放在每个季节都减少了O₃的生成（冬季、春季、夏季和秋季分别高达1.02 ppb、3.22 ppb、5.30 ppb和1.58 ppb），而在冬季促进了SOA的形成（0.01 μg/m³），在夏季则受到抑制（0.01 μg/m³）。我们还发现，在冬季高污染事件下，由于ClNO化学（非均相反应），海洋含氯物种排放可使SOA的形成增加高达0.11 μg/m³。我们的研究为NCP地区SOA形成的SSA贡献提供了新的视角。
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