Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 120, Issue 3, Pages 1778-1784Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.5b12012
Keywords
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, and Catalysis Science Program [DE-SC0012704]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
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The role of the interface between a metal and oxide (CeOx-Cu and ZnO-Cu) is critical to the production of methanol through the hydrogenation of CO2 (CO2 + 3H(2) -> CH3OH + H2O). The deposition of nanoparticles of CeOx or ZnO on Cu(111), theta(oxi) < 0.3 monolayer, produces highly active catalysts for methanol synthesis. The catalytic activity of these systems increases in the sequence: Cu(111) < ZnO/Cu(111) < CeOx/Cu(111). The apparent activation energy for the CO2 CH3OH conversion decreases from 25 kcal/mol on Cu(111) to 16 kcal/mol on ZnO/Cu(111) and 13 kcal/mol on CeOx/Cu(111). The surface chemistry of the highly active CeOx-Cu(111) interface was investigated using ambient pressure X-ray photoemission spectroscopy (AP-XPS) and infrared reflection absorption spectroscopy (AP-IRRAS). Both techniques point to the formation of formates (HCOO) and carboxylates (CO2 delta-) during the reaction. Our results show an active state of the catalyst rich in Ce3+ sites which stabilize a CO2 delta- species that is an essential intermediate for the production of methanol. The inverse oxide/metal configuration favors strong metaloxide interactions and makes possible reaction channels not seen in conventional metal/oxide catalysts.
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