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Brown carbon: An underlying driving force for rapid atmospheric sulfate formation and haze event

Journal 2020 · IF 6.551 · 发表于 2020 年 5 月 13 日
作者: Yangyang Liu,Tao Wang,Xiaozhong Fang,Yue Deng,Hanyun Cheng,Aziz-Ur-Rahim Bacha,Iqra Nabi,Liwu Zhang
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摘要

The rapid sulfate formation is a crucial factor determining the explosive growth of fine particles and the frequent occurrence of severe haze events in China. Recent field observations also show that brown carbon is one of the most critical components in aerosol particles sampled during haze episodes. To this day, there is limited knowledge that accesses the role of brown carbon in atmospheric chemistry . In fact, these carbonaceous particulate matters , mainly derived from forest fires, biomass burning , and biogenic release, can act as photosensitizers and produce varieties of active intermediates to alter oxidation capacity. Experimental results in this work provide evidence that hydroxyl radical (∙OH) stems from brown carbon proxies fulvic acid /humic acid (FA/HA) upon irradiation, leading to rapid SO 2 oxidation on brown carbon particles in the atmosphere. Further correlation analyses for sulfate formation and chromophore properties of 12 model compounds demonstrate that brown carbon particles with higher aromaticity and E 2 /E 3 (the ratio of absorbance at 254 nm to that at 365 nm) would facilitate ∙OH production and SO 2 photo-oxidation. Uptake coefficient measurements and sulfate production rate estimation indicate that brown carbon could gain importance in atmospheric SO 2 oxidation. A better understanding of SO 2 uptake kinetics on brown carbon surfaces favors in defining new regulations to improve air quality and reduce the harmful effects of haze events on resident health and the environment.

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