期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 10, 期 21, 页码 6478-6483出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b02567
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资金
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program, Project SURFACE [717022]
- Academy of Finland [308238, 314175]
- European Union [764991]
- Academy of Finland (AKA) [308238, 314175, 314175, 308238] Funding Source: Academy of Finland (AKA)
Dimethyl sulfide (DMS), produced by marine organisms, represents the most abundant, biogenic sulfur emission into the Earth's atmosphere. The gas-phase degradation of DMS is mainly initiated by the reaction with the OH radical forming first CH3SCH2O2 radicals from the dominant H-abstraction channel. It is experimentally shown that these peroxy radicals undergo a two-step isomerization process finally forming a product consistent with the formula HOOCH2SCHO. The isomerization process is accompanied by OH recycling. The rate-limiting first isomerization step, CH3SCH2O2 -> CH2SCH2OOH, followed by O-2 addition, proceeds with k = (0.23 +/- 0.12) s(-1) at 295 +/- 2 K. Competing bimolecular CH3SCH2O2 reactions with NO, HO2, or RO2 radicals are less important for trace-gas conditions over the oceans. Results of atmospheric chemistry simulations demonstrate the predominance (>= 95%) of CH3SCH2O2 isomerization. The rapid peroxy radical isomerization, not yet considered in models, substantially changes the understanding of DMS's degradation processes in the atmosphere.
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