Theoretically predicted innovative palladium stripe dopingcobalt (1 1 1) surface with excellent catalytic performance for carbon monoxide oxidative coupling to dimethyl oxalate

doi:10.1016/j.cjche.2024.03.032

中国化学工程学报 ›› 2024, Vol. 73 ›› Issue (9): 235-243.DOI: 10.1016/j.cjche.2024.03.032

Theoretically predicted innovative palladium stripe dopingcobalt (1 1 1) surface with excellent catalytic performance for carbon monoxide oxidative coupling to dimethyl oxalate

Bingying Han¹, Neng Shi¹, Mengjie Dong^1,2, Ye Liu¹, Runping Ye³, Lixia Ling², Riguang Zhang¹, Baojun Wang^1,2,4

1. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China;
2. College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China;
3. College of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China;
4. Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030013, China

收稿日期:2023-06-14 修回日期:2024-03-06 接受日期:2024-03-06 出版日期:2024-11-21 发布日期:2024-05-25
通讯作者: Lixia Ling,E-mail:linglixia@tyut.edu.cn;Baojun Wang,E-mail:wbj@tyut.edu.cn
基金资助:
This work was financially supported by the National Key Research and Development Program of China (2021YFA1502804), the Regional Innovation and Development Joint Fund of the National Natural Science Foundation of China (U22A20430), the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering (2022SX-FR001), the Natural Science Foundation of Shanxi Province (202203021212201), the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi, and the Foundation of Taiyuan University of Technology (2022QN138).

Theoretically predicted innovative palladium stripe dopingcobalt (1 1 1) surface with excellent catalytic performance for carbon monoxide oxidative coupling to dimethyl oxalate

Bingying Han¹, Neng Shi¹, Mengjie Dong^1,2, Ye Liu¹, Runping Ye³, Lixia Ling², Riguang Zhang¹, Baojun Wang^1,2,4

1. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China;
2. College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China;
3. College of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China;
4. Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030013, China

Received:2023-06-14 Revised:2024-03-06 Accepted:2024-03-06 Online:2024-11-21 Published:2024-05-25
Contact: Lixia Ling,E-mail:linglixia@tyut.edu.cn;Baojun Wang,E-mail:wbj@tyut.edu.cn
Supported by:
This work was financially supported by the National Key Research and Development Program of China (2021YFA1502804), the Regional Innovation and Development Joint Fund of the National Natural Science Foundation of China (U22A20430), the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering (2022SX-FR001), the Natural Science Foundation of Shanxi Province (202203021212201), the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi, and the Foundation of Taiyuan University of Technology (2022QN138).

摘要/Abstract

摘要： Pd-based catalysts are extensively employed to catalyze CO oxidative coupling to generate DMO, while the expensive price and high usage of Pd hinder its massive application in industrial production. Designing Pd-based catalysts with high efficiency and low Pd usage as well as expounding the catalytic mechanisms are significant for the reaction. In this study, we theoretically predict that Pd stripe doping Co(1 1 1) surface exhibits excellent performance than pure Pd(1 1 1), Pd monolayer supporting on Co(1 1 1) and Pd single atom doping Co(1 1 1) surface, and clearly expound the catalytic mechanisms through the density functional theory (DFT) calculation and micro-reaction kinetic model analysis. It is obtained that the favorable reaction pathway is COOCH₃-COOCH₃ coupling pathway over these four catalysts, while the rate-controlling step is COOCH₃+CO+OCH₃→2COOCH₃ on Pd stripe doping Co(1 1 1) surface, which is different from the case (2COOCH₃→DMO) on pure Pd(1 1 1), Pd monolayer supporting on Co(1 1 1) and Pd single atom doping Co(1 1 1) surface. This study can contribute a certain reference value for developing Pd-based catalysts with high efficiency and low Pd usage for CO oxidative coupling to DMO.

关键词: CO oxidative coupling to DMO, Pd stripe doping Co(1 1 1) surface, Catalytic mechanism, DFT calculation, Micro-reaction kinetic model analysis, Catalytic performance

Abstract: Pd-based catalysts are extensively employed to catalyze CO oxidative coupling to generate DMO, while the expensive price and high usage of Pd hinder its massive application in industrial production. Designing Pd-based catalysts with high efficiency and low Pd usage as well as expounding the catalytic mechanisms are significant for the reaction. In this study, we theoretically predict that Pd stripe doping Co(1 1 1) surface exhibits excellent performance than pure Pd(1 1 1), Pd monolayer supporting on Co(1 1 1) and Pd single atom doping Co(1 1 1) surface, and clearly expound the catalytic mechanisms through the density functional theory (DFT) calculation and micro-reaction kinetic model analysis. It is obtained that the favorable reaction pathway is COOCH₃-COOCH₃ coupling pathway over these four catalysts, while the rate-controlling step is COOCH₃+CO+OCH₃→2COOCH₃ on Pd stripe doping Co(1 1 1) surface, which is different from the case (2COOCH₃→DMO) on pure Pd(1 1 1), Pd monolayer supporting on Co(1 1 1) and Pd single atom doping Co(1 1 1) surface. This study can contribute a certain reference value for developing Pd-based catalysts with high efficiency and low Pd usage for CO oxidative coupling to DMO.

Key words: CO oxidative coupling to DMO, Pd stripe doping Co(1 1 1) surface, Catalytic mechanism, DFT calculation, Micro-reaction kinetic model analysis, Catalytic performance

Bingying Han, Neng Shi, Mengjie Dong, Ye Liu, Runping Ye, Lixia Ling, Riguang Zhang, Baojun Wang. Theoretically predicted innovative palladium stripe dopingcobalt (1 1 1) surface with excellent catalytic performance for carbon monoxide oxidative coupling to dimethyl oxalate[J]. 中国化学工程学报, 2024, 73(9): 235-243.

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Theoretically predicted innovative palladium stripe dopingcobalt (1 1 1) surface with excellent catalytic performance for carbon monoxide oxidative coupling to dimethyl oxalate

Theoretically predicted innovative palladium stripe dopingcobalt (1 1 1) surface with excellent catalytic performance for carbon monoxide oxidative coupling to dimethyl oxalate

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