期刊
CHEMCATCHEM
卷 5, 期 12, 页码 3690-3699出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201300365
关键词
density functional calculations; kinetics; platinum; reaction mechanisms; rhenium
资金
- Institute for Atom-efficient Chemical Transformations (IACT)
- Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences
- Department of Energy's Office of Biological and Environmental Research located at PNNL
- U.S. Department of Energy, Office of Science [DE-AC02-06CH11357, DEAC05-00OR22725, DE-AC02-05CH11231]
Periodic, self-consistent density functional theory calculations (DFT-GGA-PW91) on Pt(111) and Pt3Re(111) surfaces, reaction kinetics measurements, and microkinetic modeling are employed to study the mechanism of the water-gas shift (WGS) reaction over Pt and Pt-Re catalysts. The values of the reaction rates and reaction orders predicted by the model are in agreement with the ones experimentally determined; the calculated apparent activation energies are matched to within 6% of the experimental values. The primary reaction pathway is predicted to take place through adsorbed carboxyl (COOH) species, whereas formate (HCOO) is predicted to be a spectator species. We conclude that the clean Pt(111) is a good representation of the active site for the WGS reaction on Pt catalysts, whereas the active sites on the Pt-Re alloy catalyst likely contain partially oxidized metal ensembles.
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