TY - JOUR
T1 - Directional Proton Transfer in the Reaction of the Simplest Criegee Intermediate with Water Involving the Formation of Transient H3O+
AU - Liu, Jinfeng
AU - Liu, Yanqing
AU - Yang, Jinrong
AU - Zeng, Xiao Cheng
AU - He, Xiao
N1 - Funding Information:
X.H. and J.L. were supported by the National Natural Science Foundation of China (Grant Nos. 21703289, 21922301, 21761132022, and 21673074), the National Key R&D Program of China (Grant Nos. 2019YFA090402, 2016YFA0501700, and 2019YFA0905201), Shanghai Municipal Natural Science Foundation (Grant No. 18ZR1412600), “Double First-Class” University project (CPU2018GY09), the Fundamental Research Funds for China Pharmaceutical University (2632019FY01), and the Fundamental Research Funds for the Central Universities. We thank the Supercomputer Center of East China Normal University (ECNU Multifunctional Platform for Innovation 001) and China Pharmaceutical University for providing computer resources.
Funding Information:
X.H. and J.L. were supported by the National Natural Science Foundation of China (Grant Nos. 21703289, 21922301, 21761132022 and 21673074), the National Key R&D Program of China (Grant Nos. 2019YFA090402, 2016YFA0501700, and 2019YFA0905201), Shanghai Municipal Natural Science Foundation (Grant No. 18ZR1412600), "Double First-Class" University project (CPU2018GY09), the Fundamental Research Funds for China Pharmaceutical University (2632019FY01) and the Fundamental Research Funds for the Central Universities. We thank the Supercomputer Center of East China Normal University (ECNU Multifunctional Platform for Innovation 001) and China Pharmaceutical University for providing computer resources.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/4/8
Y1 - 2021/4/8
N2 - 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.
AB - 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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U2 - 10.1021/acs.jpclett.1c00448
DO - 10.1021/acs.jpclett.1c00448
M3 - Article
C2 - 33784110
AN - SCOPUS:85104047004
SN - 1948-7185
VL - 12
SP - 3379
EP - 3386
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 13
ER -