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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MDPI AG
2023-01-01
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| Series: | Symmetry |
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| Online Access: | https://www.mdpi.com/2073-8994/15/2/256 |
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| author | Zhao Tu Jiaqi Li Yan Wang Hongwei Song |
| author_facet | Zhao Tu Jiaqi Li Yan Wang Hongwei Song |
| author_sort | Zhao Tu |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-03-11T08:04:46Z |
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| institution | Directory Open Access Journal |
| issn | 2073-8994 |
| language | English |
| last_indexed | 2024-03-11T08:04:46Z |
| publishDate | 2023-01-01 |
| publisher | MDPI AG |
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| series | Symmetry |
| spelling | doaj.art-4a4c75d744704190af07570089c324d02023-11-16T23:30:53ZengMDPI AGSymmetry2073-89942023-01-0115225610.3390/sym15020256Quasi-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 ExperimentZhao Tu0Jiaqi Li1Yan Wang2Hongwei Song3School of Chemical and Environmental Engineering, Hubei Minzu University, Enshi 445000, ChinaState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, ChinaSchool of Chemical and Environmental Engineering, Hubei Minzu University, Enshi 445000, ChinaState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, ChinaThe 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.https://www.mdpi.com/2073-8994/15/2/256hydrogen abstractionenergy disposalOH + H<sub>2</sub>S reactionisotopic substitutionpotential energy surface |
| spellingShingle | Zhao Tu Jiaqi Li Yan Wang Hongwei Song 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 Symmetry hydrogen abstraction energy disposal OH + H<sub>2</sub>S reaction isotopic substitution potential energy surface |
| title | 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 |
| title_full | 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 |
| title_fullStr | 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 |
| title_full_unstemmed | 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 |
| title_short | 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 |
| title_sort | 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 |
| topic | hydrogen abstraction energy disposal OH + H<sub>2</sub>S reaction isotopic substitution potential energy surface |
| url | https://www.mdpi.com/2073-8994/15/2/256 |
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