A Highly Active Molybdenum Carbide Catalyst with Dynamic Carbon Flux for Reverse Water-Gas Shift Reaction

被引：5

作者：

Zhang, Mengtao ^{[1
]}

Zhu, Yuchen ^{[4
]}

Yan, Jie ^{[1
]}

Xie, Junzhong ^{[1
]}

Yu, Tao ^{[5
]}

Peng, Mi ^{[1
]}

Zhao, Jiayun ^{[1
]}

Xu, Yao ^{[1
]}

Li, Aowen ^{[2
,3
]}

Jia, Chunjiang ^{[6
]}

He, Lin ^{[7
]}

Wang, Meng ^{[1
]}

Zhou, Wu ^{[2
,3
]}

Wang, Rongming ^{[4
]}

Jiang, Hong ^{[1
]}

Shi, Chuan ^{[5
]}

Rodriguez, Jose ^{[8
]}

Ma, Ding ^{[1
]}

机构：

[1] Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, New Cornerstone Lab, Beijing 100871, Peoples R China

[2] Univ Chinese Acad Sci, Sch Phys Sci, Beijing 100049, Peoples R China

[3] Univ Chinese Acad Sci, CAS Key Lab Vacuum Phys, Beijing 100049, Peoples R China

[4] Univ Sci & Technol Beijing, State Key Lab Adv Met & Mat, Beijing 100083, Peoples R China

[5] Dalian Univ Technol, Coll Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China

[6] Shandong Univ, Sch Chem & Chem Engn, Key Lab Colloid & Interface Chem, Key Lab Special Aggregated Mat, Jinan 250100, Peoples R China

[7] Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Lanzhou Inst Chem Phys LICP, Lanzhou 730000, Peoples R China

[8] Brookhaven Natl Lab, Chem Div, Bldg 555, POB 5000, Upton, NY 11973 USA

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2025年 / 64卷 / 06期

基金：

中国国家自然科学基金;

关键词：

CO2; HYDROGENATION; METHANATION; REDUCTION; SUPPORTS; CERIA; MOC;

D O I：

10.1002/anie.202418645

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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 mu m olCO2/gcat/s ${{\rm { o}}{{\rm { l}}}_{{\rm { C}}{{\rm { O}}}_{{\rm { 2}}}}{\rm { /}}{{\rm { g}}}_{{\rm { cat}}}{\rm { /s}}}$ 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 alpha-MoC bulk phase and the gas phase reactants under the RWGS reaction atmosphere. This circulation, essential to maintaining the structural stability of the metastable alpha-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.

引用

页数：8

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