True Nature of the Transition-Metal Carbide/Liquid Interface Determines Its Reactivity
| Autor: | Haobo Li, Julia Kunze-Liebhäuser, Karsten Reuter, David Egger, Andreas Steiger-Thirsfeld, Eva-Maria Wernig, Niusha Shakibi Nia, Thomas Götsch, Christoph Griesser, Thomas Mairegger, Christoph Scheurer, Simon Penner, Thomas Schachinger, Dominik Wielend, Daniel Winkler |
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| Rok vydání: | 2021 |
| Předmět: |
transition-metal carbides
ab initio thermodynamics Materials science Standard hydrogen electrode Electrolyte surface Pourbaix diagram 010402 general chemistry Electrocatalyst 01 natural sciences Catalysis Carbide XPS electrocatalysis Reactivity (chemistry) Electrochemical reduction of carbon dioxide 010405 organic chemistry HER General Chemistry ddc 0104 chemical sciences solid/liquid interface Chemical physics Density functional theory electrochemical CO2 reduction Research Article |
| Zdroj: | ACS Catalysis |
| ISSN: | 2155-5435 |
| DOI: | 10.1021/acscatal.1c00415 |
| Popis: | Compound materials, such as transition-metal (TM) carbides, are anticipated to be effective electrocatalysts for the carbon dioxide reduction reaction (CO2RR) to useful chemicals. This expectation is nurtured by density functional theory (DFT) predictions of a break of key adsorption energy scaling relations that limit CO2RR at parent TMs. Here, we evaluate these prospects for hexagonal Mo2C in aqueous electrolytes in a multimethod experiment and theory approach. We find that surface oxide formation completely suppresses the CO2 activation. The oxides are stable down to potentials as low as −1.9 V versus the standard hydrogen electrode, and solely the hydrogen evolution reaction (HER) is found to be active. This generally points to the absolute imperative of recognizing the true interface establishing under operando conditions in computational screening of catalyst materials. When protected from ambient air and used in nonaqueous electrolyte, Mo2C indeed shows CO2RR activity. |
| Databáze: | OpenAIRE |
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