Quasi-Classical Trajectory Dynamics Study of the Reaction OH + H<sub>2</sub>S→H<sub>2</sub>O + SH and Its Isotopic Variants: Comparison with Experiment

The hydrogen abstraction reaction OH + H<sub>2</sub>S→H<sub>2</sub>O + SH plays an important role in acid rain formation, air pollution and climate change. In this work, the product energy disposals of the reaction and its isotopic variants OD + H<sub>2</sub>S and...

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Bibliographic Details
Main Authors: Zhao Tu, Jiaqi Li, Yan Wang, Hongwei Song
Format: Article
Language:English
Published: MDPI AG 2023-01-01
Series:Symmetry
Subjects:
Online Access:https://www.mdpi.com/2073-8994/15/2/256
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Summary:The hydrogen abstraction reaction OH + H<sub>2</sub>S→H<sub>2</sub>O + SH plays an important role in acid rain formation, air pollution and climate change. In this work, the product energy disposals of the reaction and its isotopic variants OD + H<sub>2</sub>S and OD + D<sub>2</sub>S are calculated on a new ab-initio-based ground electronic state potential energy surface (PES) using the quasi-classical trajectory method. The PES is developed by fitting a total of 72,113 points calculated at the level of UCCSD(T)-F12a/aug-cc-pVTZ and using the fundamental invariant-neural network method, resulting in a total RMSE of 4.14 meV. The product H<sub>2</sub>O formed in the OH + H<sub>2</sub>S reaction at 298 K is found to be largely populated in the first overtone states of its symmetric and asymmetric stretching modes, while the vibrational distributions of the products HOD and D<sub>2</sub>O in the isotopically substituted reactions are visibly different. The computed product vibrational state distributions agree reasonably well with experimental results and are rationalized by the sudden vector projection model.
ISSN:2073-8994