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还原态硫化合物气相氧化直接生成硫酸。

Direct sulfuric acid formation from the gas-phase oxidation of reduced-sulfur compounds.

作者信息

Berndt Torsten, Hoffmann Erik H, Tilgner Andreas, Stratmann Frank, Herrmann Hartmut

机构信息

Atmospheric Chemistry Department (ACD), Leibniz Institute for Tropospheric Research (TROPOS), 04318, Leipzig, Germany.

Atmospheric Microphysics Department (AMP), Leibniz Institute for Tropospheric Research (TROPOS), 04318, Leipzig, Germany.

出版信息

Nat Commun. 2023 Aug 10;14(1):4849. doi: 10.1038/s41467-023-40586-2.

Abstract

Sulfuric acid represents a fundamental precursor for new nanometre-sized atmospheric aerosol particles. These particles, after subsequent growth, may influence Earth´s radiative forcing directly, or indirectly through affecting the microphysical and radiative properties of clouds. Currently considered formation routes yielding sulfuric acid in the atmosphere are the gas-phase oxidation of SO initiated by OH radicals and by Criegee intermediates, the latter being of little relevance. Here we report the observation of immediate sulfuric acid production from the OH reaction of emitted organic reduced-sulfur compounds, which was speculated about in the literature for decades. Key intermediates are the methylsulfonyl radical, CHSO, and, even more interestingly, its corresponding peroxy compound, CHSOOO. Results of modelling for pristine marine conditions show that oxidation of reduced-sulfur compounds could be responsible for up to ∼50% of formed gas-phase sulfuric acid in these areas. Our findings provide a more complete understanding of the atmospheric reduced-sulfur oxidation.

摘要

硫酸是新型纳米级大气气溶胶颗粒的一种基本前体。这些颗粒在随后的生长过程中,可能直接影响地球的辐射强迫,或者通过影响云的微物理和辐射特性间接产生影响。目前认为大气中产生硫酸的形成途径是由羟基自由基和克里吉中间体引发的二氧化硫气相氧化,后者的相关性较小。在这里,我们报告了从排放的有机还原硫化合物的羟基反应中直接产生硫酸的观测结果,这在文献中已被推测了数十年。关键中间体是甲基磺酰基自由基(CH₃SO₂),甚至更有趣的是,其相应的过氧化合物(CH₃SO₃O)。原始海洋条件下的模拟结果表明,还原硫化合物的氧化可能导致这些区域中高达约50%的气相硫酸形成。我们的研究结果为大气中还原硫氧化提供了更全面的理解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9861/10415363/1ce5a0f6cf88/41467_2023_40586_Fig1_HTML.jpg

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