近日，广东工业大学环境健康与污染控制研究院、环境科学与工程学院安太成教授团队在大气有机胺非均相氧化及其辐射强迫效应影响方面取得重要进展。研究成果以“Cooling radiative forcing effect enhancement of atmospheric amines-mineral particle caused by heterogeneous uptake and oxidation (https://egusphere.copernicus.org/preprints/2024/egusphere-2024-1048/)为题发表在Atmospheric Chemistry and Physics (2024, 24(16), 9019–9030)”期刊上。论文主要作者为我院张维娜副教授和硕士生麦建铧等，通讯作者为安太成教授。

论文网址：https://egusphere.copernicus.org/preprints/2024/egusphere-2024-1048/

中文摘要：

本研究利用多种理论化学计算方法，系统揭示了有机胺类污染物在矿物表面发生非均相氧化反应机制，并在此基础上评估了其对有机胺和矿物混合态颗粒辐射强迫效应的影响。结果表明三种有机胺均能够从气相迁移到矿物表面累积，并形成有机胺和矿物混合态颗粒物，进而在大气羟基自由基的诱导下发生非均相氧化反应。进一步发现在污染大气环境下，有机胺主要进行提氢-加成氧化反应，转化成低含氧量产物RNCHO；然而在洁净大气环境下，有机胺将进行自氧化反应，则可以转化成高含氧量产物R-NCH₂OOH或R-NCH₂OOOH。两种氧化机制均能导致有机胺和矿物混合态颗粒物的光散射系数有所增加，且自氧化作用下增幅更大，由此引发的辐射强迫效应的上升幅度也更高。因此，在洁净大气环境下，有机胺氧化后的混合态颗粒物将表现出更强的制冷效应。本论文得到的该结论可在一定程度上推广至其它易进行自氧化反应的人为源有机物的混合态颗粒物体系，将为正确评估有机胺及其它人为源有机污染物形成的混合态颗粒物的辐射强迫效应的演化提供重要参考。

图文摘要

英文摘要：

Warming radiative forcing effect (RFE) derived from atmospheric amines attracts lots of attentions because of their contributions to brown carbons. Herein, the enhanced influence of amines (methyl-, dimethyl-, and trimethylamine) on cooling RFE of mineral particles is first confirmed at visible wavelengths. Present results state heterogeneous uptake and oxidation reactions of atmospheric amines are feasible on mineral particle at clean/polluted conditions, which are proofed by related thermodynamics and kinetics data obtained using combined classical molecular dynamics and density function theory methods. Based on mineral particles, simple forcing efficiency (SFE) results explain that amine uptake induces at least 11.8% – 29.5% enhancement on cooling RFE of amine-mineral particles at visible wavelengths. After amines’ heterogeneous oxidation, oxidized amine-mineral particles’ cooling RFE are furthermore enhanced due to increased oxygen contents. Moreover, oxidized amine-mineral particles under clean condition shows 27.1% – 47.1% SFE increment at 400-600 nm, which is at least 11.3% higher than that of itself under polluted condition, due to high-oxygen-content product formation through amine autoxidation. Our results suggest cooling RFE derived from atmospheric amines can be equally important to their warming RFE on atmosphere. It is necessary to update heterogeneous oxidation mechanism and kinetics data of amines in atmospheric model in order to accurately evaluate the whole RFE caused by amines on atmosphere.

资助项目：本研究受到国家自然科学基金（42020104001, 41907184和42007327），广东省基础研究和应用基础研究基金项目（2021A1515011252），广东省本土创新团队项目（2017BT01Z032）的资助。