Insights into Syngas to Methanol Conversion on Cr<sub>2</sub>O<sub>3</sub> Oxide from First-Principles-based Microkinetic Simulations

Wen-De Hu; Jun Ke; Yang-Dong Wang; Chuan-Ming Wang; Wei-Min Yang

doi:10.1063/1674-0068/cjcp2204066

Volume 35 Issue 4

Aug. 2022

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Article Navigation > Chinese Journal of Chemical Physics > 2022 > 35(4): 655-663

Wen-De Hu, Jun Ke, Yang-Dong Wang, Chuan-Ming Wang, Wei-Min Yang. Insights into Syngas to Methanol Conversion on Cr2O3 Oxide from First-Principles-based Microkinetic Simulations[J]. Chinese Journal of Chemical Physics , 2022, 35(4): 655-663. doi: 10.1063/1674-0068/cjcp2204066

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Wen-De Hu, Jun Ke, Yang-Dong Wang, Chuan-Ming Wang, Wei-Min Yang. Insights into Syngas to Methanol Conversion on Cr₂O₃ Oxide from First-Principles-based Microkinetic Simulations[J]. Chinese Journal of Chemical Physics , 2022, 35(4): 655-663. doi: 10.1063/1674-0068/cjcp2204066

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Insights into Syngas to Methanol Conversion on Cr₂O₃ Oxide from First-Principles-based Microkinetic Simulations

doi: 10.1063/1674-0068/cjcp2204066

Engineering and Industrial Catalysis, Sinopec Shanghai Research Institute of Petrochemical Technology, Shanghai 201208, China

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Corresponding author: Chuan-Ming Wang, E-mail: wangcm.sshy@sinopec.com; Wei-Min Yang, E-mail: yangwm.sshy@sinopec.com
Received Date: 2022-04-18
Accepted Date: 2022-06-22
Publish Date: 2022-08-27

Abstract

Abstract

Cr$ _2 $O$ _3 $ has been recognized as a key oxide component in bifunctional catalysts to produce bridging intermediate, e.g., methanol, from syngas. By combining density functional theory calculations and microkinetic modeling, we computationally studied the surface structures and catalytic activities of bare Cr$ _2 $O$ _3 $ (001) and (012) surfaces, and two reduced (012) surfaces covered with dissociative hydrogens or oxygen vacancies. The reduction of (001) surface is much more difficult than that of (012) surface. The stepwise or the concerted reaction pathways were explored for the syngas to methanol conversion, and the hydrogenation of CO or CHO is identified as rate-determining step. Microkinetic modeling reveals that (001) surface is inactive for the reaction, and the rates of both reduced (012) surfaces (25-28 s$ ^{-1} $) are about five times higher than bare (012) surface (4.3 s$ ^{-1} $) at 673 K. These theoretical results highlight the importance of surface reducibility on the reaction and may provide some implications on the design of individual component in bifunctional catalysis.
- Syngas to methanol,
- Cr₂O₃ oxide,
- Surface structure,
- Density functional theory calculation,
- Microkinetic modeling

^† Part of Special Topic "the 1st Young Scientist Symposium on Computational Catalysis".

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References(56)

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