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Title: A Cu/Pt Near-Surface Alloy for Water-Gas Shift Catalysis.

Abstract

The research described in this product was performed in part in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. The primary route to hydrogen production from fossil fuels involves the water-gas shift (WGS) reaction, and an improvement in the efficiency of WGS catalysts could therefore lead to a major leap forward in the realization of hydrogen economy. On the basis of a combination of high-resolution scanning tunneling microscopy, X-ray photoelectron spectroscopy, and density functional theory (DFT) calculations, we suggest the existence of a new thermodynamically stable Cu/Pt near-surface alloy (NSA). Temperature-programmed desorption and DFT reveal that this Cu/Pt NSA binds CO significantly more weakly than does Pt alone, thereby implying a considerable reduction in the potential for CO poisoning of the Cu/Pt NSA surface as compared to that of pure Pt. In addition, DFT calculations show that this Cu/Pt NSA is able to activate H2O easily, which is the rate-determining step for the WGS on several metal surfaces, and, at the same time, to bind the products of that reaction and formate intermediates rather weakly, thus avoiding possible poisoningmore » of the catalyst surface. The Cu/Pt NSA is thus a promising candidate for an improved WGS catalyst.« less

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
989063
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of the American Chemical Society, 129(20):6485-6490; Journal Volume: 129; Journal Issue: 20
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 29 ENERGY PLANNING, POLICY AND ECONOMY; ALLOYS; CATALYSIS; CATALYSTS; DESORPTION; EFFICIENCY; FORMATES; FOSSIL FUELS; FUNCTIONALS; HYDROGEN; HYDROGEN PRODUCTION; POISONING; SCANNING TUNNELING MICROSCOPY; WATER GAS; X-RAY PHOTOELECTRON SPECTROSCOPY; Environmental Molecular Sciences Laboratory

Citation Formats

Knudsen, Jan, Nilekar, Anand U., Vang, Ronnie T., Schnadt, Joachim, Kunkes, Edward L., Dumesic, James A., Mavrikakis, Manos, and Besenbacher, Fleming. A Cu/Pt Near-Surface Alloy for Water-Gas Shift Catalysis.. United States: N. p., 2007. Web. doi:10.1021/ja0700855.
Knudsen, Jan, Nilekar, Anand U., Vang, Ronnie T., Schnadt, Joachim, Kunkes, Edward L., Dumesic, James A., Mavrikakis, Manos, & Besenbacher, Fleming. A Cu/Pt Near-Surface Alloy for Water-Gas Shift Catalysis.. United States. doi:10.1021/ja0700855.
Knudsen, Jan, Nilekar, Anand U., Vang, Ronnie T., Schnadt, Joachim, Kunkes, Edward L., Dumesic, James A., Mavrikakis, Manos, and Besenbacher, Fleming. Tue . "A Cu/Pt Near-Surface Alloy for Water-Gas Shift Catalysis.". United States. doi:10.1021/ja0700855.
@article{osti_989063,
title = {A Cu/Pt Near-Surface Alloy for Water-Gas Shift Catalysis.},
author = {Knudsen, Jan and Nilekar, Anand U. and Vang, Ronnie T. and Schnadt, Joachim and Kunkes, Edward L. and Dumesic, James A. and Mavrikakis, Manos and Besenbacher, Fleming},
abstractNote = {The research described in this product was performed in part in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. The primary route to hydrogen production from fossil fuels involves the water-gas shift (WGS) reaction, and an improvement in the efficiency of WGS catalysts could therefore lead to a major leap forward in the realization of hydrogen economy. On the basis of a combination of high-resolution scanning tunneling microscopy, X-ray photoelectron spectroscopy, and density functional theory (DFT) calculations, we suggest the existence of a new thermodynamically stable Cu/Pt near-surface alloy (NSA). Temperature-programmed desorption and DFT reveal that this Cu/Pt NSA binds CO significantly more weakly than does Pt alone, thereby implying a considerable reduction in the potential for CO poisoning of the Cu/Pt NSA surface as compared to that of pure Pt. In addition, DFT calculations show that this Cu/Pt NSA is able to activate H2O easily, which is the rate-determining step for the WGS on several metal surfaces, and, at the same time, to bind the products of that reaction and formate intermediates rather weakly, thus avoiding possible poisoning of the catalyst surface. The Cu/Pt NSA is thus a promising candidate for an improved WGS catalyst.},
doi = {10.1021/ja0700855},
journal = {Journal of the American Chemical Society, 129(20):6485-6490},
number = 20,
volume = 129,
place = {United States},
year = {Tue May 01 00:00:00 EDT 2007},
month = {Tue May 01 00:00:00 EDT 2007}
}