A Highly Active Molybdenum Carbide Catalyst with Dynamic Carbon Flux for Reverse Water‐Gas Shift Reaction
Molybdenum carbide has been reported as an efficient and stable catalyst for reverse water-gas shift (RWGS) reaction. The conventional understanding of the mechanism suggests domination of the surface phenomena, with only surface or subsurface layers partaking in the catalytic cycle. In this study, we presented a highly active MoC catalyst from carburization process, which showed a mass-specific reaction rate over 260 μm <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:semantics><mml:mrow><mml:mi>o</mml:mi> <mml:msub><mml:mi>l</mml:mi> <mml:mrow><mml:mi>C</mml:mi> <mml:msub><mml:mi>O</mml:mi> <mml:mn>2</mml:mn></mml:msub> </mml:mrow> </mml:msub> <mml:mo>/</mml:mo> <mml:msub><mml:mi>g</mml:mi> <mml:mi>cat</mml:mi></mml:msub> <mml:mrow><mml:mo>/</mml:mo> <mml:mi>s</mml:mi></mml:mrow> </mml:mrow> <mml:annotation>${{\rm { o}}{{\rm { l}}}_{{\rm { C}}{{\rm { O}}}_{{\rm { 2}}}}{\rm { /}}{{\rm { g}}}_{{\rm { cat}}}{\rm { /s}}}$</mml:annotation> </mml:semantics> </mml:math> with dynamic carbon flux in the bulk phase of the catalyst. Through Isotopic Temperature-Programmed Reaction (ITPR) analysis and Environmental Transmission Electron Microscopy (ETEM), we discerned dynamic carbon flow circulating between the α-MoC bulk phase and the gas phase reactants under the RWGS reaction atmosphere. This circulation, essential to maintaining the structural stability of the metastable α-MoC and its ultra-high reactivity, is accompanied by thorough carbon component exchange among the bulk, the surface and the gas-phase reactants during the reaction process.
Authors
- Tao Yu (ORCID: https://orcid.org/0000-0001-9516-4259)
- Chuan Shi (ORCID: https://orcid.org/0000-0002-5152-7561)
- Junzhong Xie (ORCID: https://orcid.org/0000-0002-9457-9572)
- Mi Peng (ORCID: https://orcid.org/0000-0001-7713-4398)
- Meng Wang (ORCID: https://orcid.org/0000-0003-4067-1127)
- Aowen Li (ORCID: https://orcid.org/0009-0001-0975-1068)
- Rongming Wang (ORCID: https://orcid.org/0000-0003-4075-6956)
- Chun‐Jiang Jia (ORCID: https://orcid.org/0000-0002-4254-5100)
- Hong Jiang (ORCID: https://orcid.org/0000-0003-3187-2023)
- Lin He (ORCID: https://orcid.org/0000-0001-7437-1443)
- Wu Zhou (ORCID: https://orcid.org/0000-0002-9202-1989)
- José A. Rodríguez (ORCID: https://orcid.org/0000-0002-5680-4214)
- Yao Xu (ORCID: https://orcid.org/0009-0006-4823-2187)
- Yuchen Zhu (ORCID: https://orcid.org/0000-0002-7204-2985)
- J. Zhao (ORCID: https://orcid.org/0000-0003-0966-4850)
- Jie Yan (ORCID: https://orcid.org/0000-0002-2326-977X)
- Mengtao Zhang (ORCID: https://orcid.org/0000-0002-4152-1019)
- Ding Ma (ORCID: https://orcid.org/0000-0002-3341-2998)
Institutions
- Shandong University (CN)
- Chinese Academy of Sciences (CN)
- Brookhaven National Laboratory (US)
- Peking University (CN)
- Dalian University of Technology (CN)
- University of Jinan (CN)
- Lanzhou Institute of Chemical Physics (CN)
- Dalian University (CN)
- Beijing National Laboratory for Molecular Sciences (CN)
- University of Chinese Academy of Sciences (CN)
- University of Science and Technology Beijing (CN)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2024-12-07
- DOI
- https://doi.org/10.1002/anie.202418645
- Citations
- 20
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 2.34
Funders
- Salt Science Research Foundation
- Tencent
- National Natural Science Foundation of China
- National Key Research and Development Program of China
- Argonne National Laboratory