期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 7, 期 22, 页码 5332-5342出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7cy00639j
关键词
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资金
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences [DE-SC0012704]
- BID
- MINECO/FEDER [CTQ2015-64618-R]
- Generalitat de Catalunya [2014SGR97]
- NOMAD Center of Excellence project
- European Union Horizon research and innovation programme [676580]
- Spanish MEC predoctoral grant [CTQ2012-30751]
- MINECO [RYC-2012-10129]
- ICREA Academia Award for Excellence in University Research
- National High Technology Research and Development Program of China [2013AA051201]
The water gas shift (WGS) reaction catalyzed by orthorhombic beta-Mo2C and cubic delta-MoC surfaces with and without Au clusters supported thereon has been studied by means of a combination of sophisticated experiments and state-of-the- art computational modeling. Experiments evidence the importance of the metal/carbon ratio on the performance of these systems, where Au/delta-MoC is presented as a suitable catalyst for WGS at low temperatures owing to its high activity, selectivity (only CO2 and H-2 are detected), and stability (oxycarbides are not observed). Periodic density functional theory-based calculations show that the supported Au clusters and the Au/delta-MoC interface do not take part directly in water dissociation but their presence is crucial to switch the reaction mechanism, drastically decreasing the effect of the reverse WGS reaction and favoring the WGS products desorption, thus leading to an increase in CO2 and H-2 production. The present results clearly display the importance of the Mo/C ratio and the synergy with the admetal clusters in tuning the activity and selectivity of the carbide substrate.
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