Reverse water gas-shift reaction product driven dynamic activation of molybdenum nitride catalyst surface

Hui Xin, Rongtan Li, Le Lin, Rentao Mu, Mingrun Li, Dan Li (), Qiang Fu () and Xinhe Bao ()
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Hui Xin: Chinese Academy of Sciences
Rongtan Li: Chinese Academy of Sciences
Le Lin: Chinese Academy of Sciences
Rentao Mu: Chinese Academy of Sciences
Mingrun Li: Chinese Academy of Sciences
Dan Li: Sichuan University
Qiang Fu: Chinese Academy of Sciences
Xinhe Bao: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract In heterogeneous catalysis catalyst activation is often observed during the reaction process, which is mostly attributed to the induction by reactants. In this work we report that surface structure of molybdenum nitride (MoNx) catalyst exhibits a high dependency on the partial pressure or concentration of reaction products i.e., CO and H2O in reverse water gas-shift reaction (RWGS) (CO2:H2 = 1:3) but not reactants of CO2 and H2. Molybdenum oxide (MoOx) overlayers formed by oxidation with H2O are observed at reaction pressure below 10 mbar or with low partial pressure of CO/H2O products, while CO-induced surface carbonization happens at reaction pressure above 100 mbar and with high partial pressure of CO/H2O products. The reaction products induce restructuring of MoNx surface into more active molybdenum carbide (MoCx) to increase the reaction rate and make for higher partial pressure CO, which in turn promote further surface carbonization of MoNx. We refer to this as the positive feedback between catalytic activity and catalyst activation in RWGS, which should be widely present in heterogeneous catalysis.

Date: 2024
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DOI: 10.1038/s41467-024-47550-8

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