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柴油机碳烟的光氧化作用增强了硫酸氢盐的非均相形成。

Diesel soot photooxidation enhances the heterogeneous formation of HSO.

作者信息

Zhang Peng, Chen Tianzeng, Ma Qingxin, Chu Biwu, Wang Yonghong, Mu Yujing, Yu Yunbo, He Hong

机构信息

State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, 100085, Beijing, China.

University of Chinese Academy of Sciences, 100049, Beijing, China.

出版信息

Nat Commun. 2022 Sep 12;13(1):5364. doi: 10.1038/s41467-022-33120-3.

Abstract

Both field observation and experimental simulation have implied that black carbon or soot plays a remarkable role in the catalytic oxidation of SO for the formation of atmospheric sulfate. However, the catalytic mechanism remains ambiguous, especially that under light irradiation. Here we systematically investigate the heterogeneous conversion of SO on diesel soot or black carbon (DBC) under light irradiation. The experimental results show that the presence of DBC under light irradiation can significantly promote the heterogeneous conversion of SO to HSO, mainly through the heterogeneous reaction between SO and photo-induced OH radicals. The detected photo-chemical behaviors on DBC suggest that OH radical formation is closely related to the abstraction and transfer of electrons in DBC and the formation of reactive superoxide radical (•O) as an intermediate. Our results extend the known sources of atmospheric HSO and provide insight into the internal photochemical oxidation mechanism of SO on DBC.

摘要

实地观测和实验模拟均表明,黑碳或烟灰在大气硫酸盐形成过程中对二氧化硫的催化氧化起着显著作用。然而,催化机制仍不明确,尤其是在光照条件下。在此,我们系统地研究了光照下二氧化硫在柴油机碳烟或黑碳(DBC)上的非均相转化。实验结果表明,光照下DBC的存在能显著促进二氧化硫向亚硫酸氢根的非均相转化,主要是通过二氧化硫与光致羟基自由基之间的非均相反应实现的。在DBC上检测到的光化学行为表明,羟基自由基的形成与DBC中电子的提取和转移以及作为中间体的活性超氧自由基(•O)的形成密切相关。我们的研究结果扩展了大气中亚硫酸氢根的已知来源,并深入了解了二氧化硫在DBC上的内部光化学氧化机制。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f627/9467980/05b5066a0589/41467_2022_33120_Fig1_HTML.jpg

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