A Cu/Pt Near-Surface Alloy for Water−Gas Shift Catalysis
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...
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| Veröffentlicht in: | Journal of the American Chemical Society 2007-05, Vol.129 (20), p.6485-6490 |
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| container_title | Journal of the American Chemical Society |
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| creator | Knudsen, Jan Nilekar, Anand U Vang, Ronnie T Schnadt, Joachim Kunkes, Edward L Dumesic, James A Mavrikakis, Manos Besenbacher, Flemming |
| description | 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_str_mv | 10.1021/ja0700855 |
| format | Article |
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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.</description><identifier>ISSN: 0002-7863</identifier><identifier>EISSN: 1520-5126</identifier><identifier>DOI: 10.1021/ja0700855</identifier><identifier>PMID: 17469820</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>08 HYDROGEN ; ALLOYS ; Alloys - chemistry ; CATALYSIS ; CATALYSTS ; Copper - chemistry ; DESORPTION ; EFFICIENCY ; ENERGY PLANNING, POLICY AND ECONOMY ; Environmental Molecular Sciences Laboratory ; FORMATES ; FOSSIL FUELS ; FUNCTIONALS ; Gases - chemistry ; HYDROGEN ; HYDROGEN PRODUCTION ; Microscopy, Scanning Tunneling ; Models, Molecular ; Molecular Conformation ; Platinum - chemistry ; POISONING ; SCANNING TUNNELING MICROSCOPY ; Surface Properties ; Water - chemistry ; WATER GAS ; X-RAY PHOTOELECTRON SPECTROSCOPY</subject><ispartof>Journal of the American Chemical Society, 2007-05, Vol.129 (20), p.6485-6490</ispartof><rights>Copyright © 2007 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a414t-711428c935e1b1ea8860dfb96211e279637be99ac1c49233c4d4f7de1d7130ba3</citedby><cites>FETCH-LOGICAL-a414t-711428c935e1b1ea8860dfb96211e279637be99ac1c49233c4d4f7de1d7130ba3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/ja0700855$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/ja0700855$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/17469820$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/989063$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Knudsen, Jan</creatorcontrib><creatorcontrib>Nilekar, Anand U</creatorcontrib><creatorcontrib>Vang, Ronnie T</creatorcontrib><creatorcontrib>Schnadt, Joachim</creatorcontrib><creatorcontrib>Kunkes, Edward L</creatorcontrib><creatorcontrib>Dumesic, James A</creatorcontrib><creatorcontrib>Mavrikakis, Manos</creatorcontrib><creatorcontrib>Besenbacher, Flemming</creatorcontrib><creatorcontrib>Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)</creatorcontrib><title>A Cu/Pt Near-Surface Alloy for Water−Gas Shift Catalysis</title><title>Journal of the American Chemical Society</title><addtitle>J. Am. Chem. Soc</addtitle><description>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.</description><subject>08 HYDROGEN</subject><subject>ALLOYS</subject><subject>Alloys - chemistry</subject><subject>CATALYSIS</subject><subject>CATALYSTS</subject><subject>Copper - chemistry</subject><subject>DESORPTION</subject><subject>EFFICIENCY</subject><subject>ENERGY PLANNING, POLICY AND ECONOMY</subject><subject>Environmental Molecular Sciences Laboratory</subject><subject>FORMATES</subject><subject>FOSSIL FUELS</subject><subject>FUNCTIONALS</subject><subject>Gases - chemistry</subject><subject>HYDROGEN</subject><subject>HYDROGEN PRODUCTION</subject><subject>Microscopy, Scanning Tunneling</subject><subject>Models, Molecular</subject><subject>Molecular Conformation</subject><subject>Platinum - chemistry</subject><subject>POISONING</subject><subject>SCANNING TUNNELING MICROSCOPY</subject><subject>Surface Properties</subject><subject>Water - chemistry</subject><subject>WATER GAS</subject><subject>X-RAY PHOTOELECTRON SPECTROSCOPY</subject><issn>0002-7863</issn><issn>1520-5126</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2007</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNpt0LFOwzAQBmALgWgpDLwACgMDQ6jPTuKYrQrQgqpSlCJGy3EcNaVtKtuR6Bsw84g8CUGpysJ0Ot2n-6UfoXPAN4AJ9BcSM4zjMDxAXQgJ9kMg0SHqYoyJz-KIdtCJtYtmDUgMx6gDLIh4THAX3Q68pO5PnTfR0vhpbQqptDdYLqutV1TGe5NOm-_Pr6G0XjovC-cl0snl1pb2FB0Vcmn12W720OvD_SwZ-ePn4WMyGPsygMD5DKBJVZyGGjLQMo4jnBcZjwiAJoxHlGWac6lABZxQqoI8KFiuIWdAcSZpD122fyvrSmFV6bSaq2q91soJHnMc0cZct0aZylqjC7Ex5UqarQAsfjsS-44ae9HaTZ2tdP4nd6U0wG9BaZ3-2N-leRcRoywUs2kqRnfJSzJ6moi08Vetl8qKRVWbdVPHP8E_Bip6EQ</recordid><startdate>20070523</startdate><enddate>20070523</enddate><creator>Knudsen, Jan</creator><creator>Nilekar, Anand U</creator><creator>Vang, Ronnie T</creator><creator>Schnadt, Joachim</creator><creator>Kunkes, Edward L</creator><creator>Dumesic, James A</creator><creator>Mavrikakis, Manos</creator><creator>Besenbacher, Flemming</creator><general>American Chemical Society</general><scope>BSCLL</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope></search><sort><creationdate>20070523</creationdate><title>A Cu/Pt Near-Surface Alloy for Water−Gas Shift Catalysis</title><author>Knudsen, Jan ; Nilekar, Anand U ; Vang, Ronnie T ; Schnadt, Joachim ; Kunkes, Edward L ; Dumesic, James A ; Mavrikakis, Manos ; Besenbacher, Flemming</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a414t-711428c935e1b1ea8860dfb96211e279637be99ac1c49233c4d4f7de1d7130ba3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2007</creationdate><topic>08 HYDROGEN</topic><topic>ALLOYS</topic><topic>Alloys - chemistry</topic><topic>CATALYSIS</topic><topic>CATALYSTS</topic><topic>Copper - chemistry</topic><topic>DESORPTION</topic><topic>EFFICIENCY</topic><topic>ENERGY PLANNING, POLICY AND ECONOMY</topic><topic>Environmental Molecular Sciences Laboratory</topic><topic>FORMATES</topic><topic>FOSSIL FUELS</topic><topic>FUNCTIONALS</topic><topic>Gases - chemistry</topic><topic>HYDROGEN</topic><topic>HYDROGEN PRODUCTION</topic><topic>Microscopy, Scanning Tunneling</topic><topic>Models, Molecular</topic><topic>Molecular Conformation</topic><topic>Platinum - chemistry</topic><topic>POISONING</topic><topic>SCANNING TUNNELING MICROSCOPY</topic><topic>Surface Properties</topic><topic>Water - chemistry</topic><topic>WATER GAS</topic><topic>X-RAY PHOTOELECTRON SPECTROSCOPY</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Knudsen, Jan</creatorcontrib><creatorcontrib>Nilekar, Anand U</creatorcontrib><creatorcontrib>Vang, Ronnie T</creatorcontrib><creatorcontrib>Schnadt, Joachim</creatorcontrib><creatorcontrib>Kunkes, Edward L</creatorcontrib><creatorcontrib>Dumesic, James A</creatorcontrib><creatorcontrib>Mavrikakis, Manos</creatorcontrib><creatorcontrib>Besenbacher, Flemming</creatorcontrib><creatorcontrib>Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)</creatorcontrib><collection>Istex</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>Journal of the American Chemical Society</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Knudsen, Jan</au><au>Nilekar, Anand U</au><au>Vang, Ronnie T</au><au>Schnadt, Joachim</au><au>Kunkes, Edward L</au><au>Dumesic, James A</au><au>Mavrikakis, Manos</au><au>Besenbacher, Flemming</au><aucorp>Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>A Cu/Pt Near-Surface Alloy for Water−Gas Shift Catalysis</atitle><jtitle>Journal of the American Chemical Society</jtitle><addtitle>J. Am. Chem. Soc</addtitle><date>2007-05-23</date><risdate>2007</risdate><volume>129</volume><issue>20</issue><spage>6485</spage><epage>6490</epage><pages>6485-6490</pages><issn>0002-7863</issn><eissn>1520-5126</eissn><abstract>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.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>17469820</pmid><doi>10.1021/ja0700855</doi><tpages>6</tpages></addata></record> |
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| subjects | 08 HYDROGEN ALLOYS Alloys - chemistry CATALYSIS CATALYSTS Copper - chemistry DESORPTION EFFICIENCY ENERGY PLANNING, POLICY AND ECONOMY Environmental Molecular Sciences Laboratory FORMATES FOSSIL FUELS FUNCTIONALS Gases - chemistry HYDROGEN HYDROGEN PRODUCTION Microscopy, Scanning Tunneling Models, Molecular Molecular Conformation Platinum - chemistry POISONING SCANNING TUNNELING MICROSCOPY Surface Properties Water - chemistry WATER GAS X-RAY PHOTOELECTRON SPECTROSCOPY |
| title | A Cu/Pt Near-Surface Alloy for Water−Gas Shift Catalysis |
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