期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 12, 期 13, 页码 3379-3386出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c00448
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资金
- National Natural Science Foundation of China [21703289, 21922301, 21761132022, 21673074]
- National Key R&D Program of China [2019YFA090402, 2016YFA0501700, 2019YFA0905201]
- Shanghai Municipal Natural Science Foundation [18ZR1412600]
- Double First-Class University project [CPU2018GY09]
- Fundamental Research Funds for China Pharmaceutical University [2632019FY01]
- Fundamental Research Funds for the Central Universities
The reaction of the smallest Criegee intermediate, CH2OO, with a water cluster was investigated through ab initio molecular dynamics simulations. The reaction was found to occur both at the air/water interface and inside the water cluster, requiring more than one reactive water molecule. Different reaction pathways were observed, with the involvement of transient H3O+ impacting the atmospheric budget of trace gases.
The reaction of Criegee intermediates with water vapor has been widely known as a key Criegee reaction in the troposphere. Herein, we investigated the reaction of the smallest Criegee intermediate, CH2OO, with a water cluster through fragment-based ab initio molecular dynamics simulations at the MP2/aug-cc-pVDZ level. Our results show that the CH2OO-water reaction could occur not only at the air/water interface but also inside the water cluster. Moreover, more than one reactive water molecules are required for the CH2OO-water reaction, which is always initiated from the Criegee carbon atom and ends at the terminal Criegee oxygen atom via a directional proton transfer process. The observed reaction pathways include the loop-structure-mediated and stepwise mechanisms, and the latter involves the formation of transient H3O+. The lifetime of transient H3O+ is on the order of a few picoseconds, which may impact the atmospheric budget of the other trace gases in the actual atmosphere.
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