Characterisation of environmentally persistent free radicals and their contributions to oxidative potential and reactive oxygen species in sea spray and size-resolved ambient particles

IF 8.5 1区地球科学 Q1 METEOROLOGY & ATMOSPHERIC SCIENCES npj Climate and Atmospheric Science Pub Date : 2025-01-21 DOI:10.1038/s41612-025-00911-6

Xinji Zhang, Fanyi Wei, Haiyan Fu, Huibin Guo

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Abstract

Aerosols, derived from natural processes and human activities, present various risks to the environment and human health. In this regard, the role of recent pollutant environmentally persistent free radicals (EPFRs) should not be overlooked. However, the oxidative toxicity and mass transfer processes of EPFRs in liquid-phase environments remain completely understood. In this study, the dispersion characteristics of EPFRs and their contributions to the oxidation potential (OP) and reactive oxygen species (ROS) in sea spray and size-resolved PM were investigated and compared. The results showed that the sea spray contained fast-decaying C-centred EPFRs with a half-life of 0.32 years. The concentration ranged from 0.3 × 10¹³ spins/m³ to 7.5 × 10¹³ spins/m³. It increased as the samples approached the coast. Moreover, the size-resolved PM contained slow-decaying O-centred EPFRs with a half-life of 0.51 years. The concentration ranged from 4.57 × 10¹³ spins/m³ to 11.46 × 10¹³ spins/m³, which was higher than that of most sea spray samples. The interaction between sea spray and water mainly generated hydroxyl free radicals (54 ± 3%), whereas the size-resolved PM mainly generated organic free radicals (64 ± 5%). Correlation analysis revealed that EPFRs may be involved in ROS generation. In addition, the mass transfer of EPFRs between the PM and sea spray may have been controlled by both gas and liquid films. The concentration of EPFRs at the phase interface was calculated to be 4.92 × 10¹³ spins/m³. In summary, EPFRs positively contribute to OP and ROS production.

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环境持久性自由基的特征及其对海洋喷雾和大小分辨环境颗粒中氧化电位和活性氧的贡献

来自自然过程和人类活动的气溶胶对环境和人类健康构成各种风险。在这方面，近期污染物环境持久性自由基（EPFRs）的作用不容忽视。然而，epfr在液相环境中的氧化毒性和传质过程仍未完全了解。本研究研究并比较了EPFRs在浪花和粒径分解PM中的分散特性及其对氧化电位（OP）和活性氧（ROS）的贡献。结果表明，海雾中含有快速衰变的c中心EPFRs，半衰期为0.32年。浓度范围为0.3 × 1013自旋/m3 ~ 7.5 × 1013自旋/m3。当样本靠近海岸时，它增加了。此外，尺寸分辨的PM含有慢衰变的o中心epfr，半衰期为0.51年。浓度范围为4.57 ~ 11.46 × 1013旋/m3，高于大部分海雾样品。浪花与水的相互作用主要产生羟基自由基（54±3%），而粒径分解PM主要产生有机自由基（64±5%）。相关分析显示EPFRs可能参与ROS的生成。此外，epfr在PM和海喷雾之间的传质可能受到气膜和液膜的控制。计算出EPFRs在相界面处的浓度为4.92 × 1013自旋/m3。综上所述，EPFRs积极促进OP和ROS的产生。

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来源期刊

npj Climate and Atmospheric Science Earth and Planetary Sciences-Atmospheric Science

CiteScore

8.80

自引率

3.30%

发文量

审稿时长

21 weeks

期刊介绍： npj Climate and Atmospheric Science is an open-access journal encompassing the relevant physical, chemical, and biological aspects of atmospheric and climate science. The journal places particular emphasis on regional studies that unveil new insights into specific localities, including examinations of local atmospheric composition, such as aerosols. The range of topics covered by the journal includes climate dynamics, climate variability, weather and climate prediction, climate change, ocean dynamics, weather extremes, air pollution, atmospheric chemistry (including aerosols), the hydrological cycle, and atmosphere–ocean and atmosphere–land interactions. The journal welcomes studies employing a diverse array of methods, including numerical and statistical modeling, the development and application of in situ observational techniques, remote sensing, and the development or evaluation of new reanalyses.