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Hydrogen Chemisorption on Silica-Supported Pt Clusters: In Situ X-ray Absorption Spectroscopy
Hydrogen chemisorption on small silica-supported Pt clusters was investigated using in situ extended X-ray absorption fine structure (EXAFS) spectroscopy and X-ray absorption near-edge structure (XANES) spectroscopy. The clusters were found to exhibit a bulklike Pt first nearest neighbor (NN) distan...
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| Published in: | The journal of physical chemistry. B 1997-06, Vol.101 (25), p.4972-4977 |
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| Main Authors: | , , , |
| Format: | Article |
| Language: | English |
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| cited_by | cdi_FETCH-LOGICAL-a227t-b7c69b6aa976b11b8e390f8c3df227e6889887b765654079eadbe4371a952df63 |
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| cites | cdi_FETCH-LOGICAL-a227t-b7c69b6aa976b11b8e390f8c3df227e6889887b765654079eadbe4371a952df63 |
| container_end_page | 4977 |
| container_issue | 25 |
| container_start_page | 4972 |
| container_title | The journal of physical chemistry. B |
| container_volume | 101 |
| creator | Reifsnyder, Scott N Otten, Mark M Sayers, Dale E Lamb, H. Henry |
| description | Hydrogen chemisorption on small silica-supported Pt clusters was investigated using in situ extended X-ray absorption fine structure (EXAFS) spectroscopy and X-ray absorption near-edge structure (XANES) spectroscopy. The clusters were found to exhibit a bulklike Pt first nearest neighbor (NN) distance (2.76 Å) and low disorder while covered by chemisorbed hydrogen. In contrast, bare Pt clusters produced by heating in vacuo at 300 °C are characterized by a contracted Pt NN distance (2.66 Å) and greater disorder. These effects are reversed by re-exposure of the bare Pt clusters to H2 at 25 °C. The metal−support interface is characterized by a short Pt−O distance, irrespective of the presence of chemisorbed hydrogen. An apparent L3 edge shift of 0.8 eV relative to bulk Pt is observed for the hydrogen-covered clusters. This shift is attributed to a decrease in the Pt L3 edge resonance (white line) intensity, as no corresponding shift is observed at the L2 edge. A hydrogen-related L2,3 XANES feature at 9 eV appears with nearly equal intensity at each edge. This peak is assigned to electronic transitions from Pt 2p levels to H 1s−Pt 5d antibonding states with mixed d3/2−d5/2 character. From the L2,3 XANES analysis, we find that the number of unoccupied d states in hydrogen-covered Pt clusters is 23% less than in bulk Pt. In contrast, the L2,3 XANES spectra of bare silica-supported Pt clusters are closely similar to those of bulk Pt; quantitative analysis reveals only a slight (4%) decrease in the number of unoccupied d states. |
| doi_str_mv | 10.1021/jp970244e |
| format | article |
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Henry</creator><creatorcontrib>Reifsnyder, Scott N ; Otten, Mark M ; Sayers, Dale E ; Lamb, H. Henry</creatorcontrib><description>Hydrogen chemisorption on small silica-supported Pt clusters was investigated using in situ extended X-ray absorption fine structure (EXAFS) spectroscopy and X-ray absorption near-edge structure (XANES) spectroscopy. The clusters were found to exhibit a bulklike Pt first nearest neighbor (NN) distance (2.76 Å) and low disorder while covered by chemisorbed hydrogen. In contrast, bare Pt clusters produced by heating in vacuo at 300 °C are characterized by a contracted Pt NN distance (2.66 Å) and greater disorder. These effects are reversed by re-exposure of the bare Pt clusters to H2 at 25 °C. The metal−support interface is characterized by a short Pt−O distance, irrespective of the presence of chemisorbed hydrogen. An apparent L3 edge shift of 0.8 eV relative to bulk Pt is observed for the hydrogen-covered clusters. This shift is attributed to a decrease in the Pt L3 edge resonance (white line) intensity, as no corresponding shift is observed at the L2 edge. A hydrogen-related L2,3 XANES feature at 9 eV appears with nearly equal intensity at each edge. This peak is assigned to electronic transitions from Pt 2p levels to H 1s−Pt 5d antibonding states with mixed d3/2−d5/2 character. From the L2,3 XANES analysis, we find that the number of unoccupied d states in hydrogen-covered Pt clusters is 23% less than in bulk Pt. In contrast, the L2,3 XANES spectra of bare silica-supported Pt clusters are closely similar to those of bulk Pt; quantitative analysis reveals only a slight (4%) decrease in the number of unoccupied d states.</description><identifier>ISSN: 1520-6106</identifier><identifier>EISSN: 1520-5207</identifier><identifier>DOI: 10.1021/jp970244e</identifier><language>eng</language><publisher>American Chemical Society</publisher><ispartof>The journal of physical chemistry. B, 1997-06, Vol.101 (25), p.4972-4977</ispartof><rights>Copyright © 1997 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a227t-b7c69b6aa976b11b8e390f8c3df227e6889887b765654079eadbe4371a952df63</citedby><cites>FETCH-LOGICAL-a227t-b7c69b6aa976b11b8e390f8c3df227e6889887b765654079eadbe4371a952df63</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>315,786,790,27957,27958</link.rule.ids></links><search><creatorcontrib>Reifsnyder, Scott N</creatorcontrib><creatorcontrib>Otten, Mark M</creatorcontrib><creatorcontrib>Sayers, Dale E</creatorcontrib><creatorcontrib>Lamb, H. Henry</creatorcontrib><title>Hydrogen Chemisorption on Silica-Supported Pt Clusters: In Situ X-ray Absorption Spectroscopy</title><title>The journal of physical chemistry. B</title><addtitle>J. Phys. Chem. B</addtitle><description>Hydrogen chemisorption on small silica-supported Pt clusters was investigated using in situ extended X-ray absorption fine structure (EXAFS) spectroscopy and X-ray absorption near-edge structure (XANES) spectroscopy. The clusters were found to exhibit a bulklike Pt first nearest neighbor (NN) distance (2.76 Å) and low disorder while covered by chemisorbed hydrogen. In contrast, bare Pt clusters produced by heating in vacuo at 300 °C are characterized by a contracted Pt NN distance (2.66 Å) and greater disorder. These effects are reversed by re-exposure of the bare Pt clusters to H2 at 25 °C. The metal−support interface is characterized by a short Pt−O distance, irrespective of the presence of chemisorbed hydrogen. An apparent L3 edge shift of 0.8 eV relative to bulk Pt is observed for the hydrogen-covered clusters. This shift is attributed to a decrease in the Pt L3 edge resonance (white line) intensity, as no corresponding shift is observed at the L2 edge. A hydrogen-related L2,3 XANES feature at 9 eV appears with nearly equal intensity at each edge. This peak is assigned to electronic transitions from Pt 2p levels to H 1s−Pt 5d antibonding states with mixed d3/2−d5/2 character. From the L2,3 XANES analysis, we find that the number of unoccupied d states in hydrogen-covered Pt clusters is 23% less than in bulk Pt. In contrast, the L2,3 XANES spectra of bare silica-supported Pt clusters are closely similar to those of bulk Pt; quantitative analysis reveals only a slight (4%) decrease in the number of unoccupied d states.</description><issn>1520-6106</issn><issn>1520-5207</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>1997</creationdate><recordtype>article</recordtype><recordid>eNptkD1PwzAQhi0EEqUw8A-8MDAEbCfxB1sVPlqpEkUpUjdjJw6ktE1kOxLZWPmb_BJcteqEdKc76Z57T-8BcInRDUYE3y5bwRBJEnMEBjglKArJjvc9xYiegjPnlgiRlHA6AG_jvrTNu9nA7MOsa9fY1tfNBobI61VdqCjv2rax3pRw5mG26pw31t39fv_AyZbxHVxEVvVwpA_LeWsKbxtXNG1_Dk4qtXLmYl-H4PXxYZ6No-nz0yQbTSNFCPORZgUVmiolGNUYa25igSpexGUV5oZyLjhnmtGUpgliwqhSmyRmWImUlBWNh-B6p1uEw86aSra2XivbS4zk9jXy8JrARju2Dma-DqCyn5KymKVyPsvl_fRlviBZKheBv9rxqnBy2XR2E5z8o_sHYRZzcg</recordid><startdate>19970619</startdate><enddate>19970619</enddate><creator>Reifsnyder, Scott N</creator><creator>Otten, Mark M</creator><creator>Sayers, Dale E</creator><creator>Lamb, H. Henry</creator><general>American Chemical Society</general><scope>BSCLL</scope><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>19970619</creationdate><title>Hydrogen Chemisorption on Silica-Supported Pt Clusters: In Situ X-ray Absorption Spectroscopy</title><author>Reifsnyder, Scott N ; Otten, Mark M ; Sayers, Dale E ; Lamb, H. Henry</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a227t-b7c69b6aa976b11b8e390f8c3df227e6889887b765654079eadbe4371a952df63</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>1997</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Reifsnyder, Scott N</creatorcontrib><creatorcontrib>Otten, Mark M</creatorcontrib><creatorcontrib>Sayers, Dale E</creatorcontrib><creatorcontrib>Lamb, H. Henry</creatorcontrib><collection>Istex</collection><collection>CrossRef</collection><jtitle>The journal of physical chemistry. B</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Reifsnyder, Scott N</au><au>Otten, Mark M</au><au>Sayers, Dale E</au><au>Lamb, H. Henry</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Hydrogen Chemisorption on Silica-Supported Pt Clusters: In Situ X-ray Absorption Spectroscopy</atitle><jtitle>The journal of physical chemistry. B</jtitle><addtitle>J. Phys. Chem. B</addtitle><date>1997-06-19</date><risdate>1997</risdate><volume>101</volume><issue>25</issue><spage>4972</spage><epage>4977</epage><pages>4972-4977</pages><issn>1520-6106</issn><eissn>1520-5207</eissn><notes>Abstract published in Advance ACS Abstracts, June 1, 1997.</notes><notes>ark:/67375/TPS-DLQTX2C5-X</notes><notes>istex:341B25D3F23A5E4B561D3C41905013C18486A40E</notes><abstract>Hydrogen chemisorption on small silica-supported Pt clusters was investigated using in situ extended X-ray absorption fine structure (EXAFS) spectroscopy and X-ray absorption near-edge structure (XANES) spectroscopy. The clusters were found to exhibit a bulklike Pt first nearest neighbor (NN) distance (2.76 Å) and low disorder while covered by chemisorbed hydrogen. In contrast, bare Pt clusters produced by heating in vacuo at 300 °C are characterized by a contracted Pt NN distance (2.66 Å) and greater disorder. These effects are reversed by re-exposure of the bare Pt clusters to H2 at 25 °C. The metal−support interface is characterized by a short Pt−O distance, irrespective of the presence of chemisorbed hydrogen. An apparent L3 edge shift of 0.8 eV relative to bulk Pt is observed for the hydrogen-covered clusters. This shift is attributed to a decrease in the Pt L3 edge resonance (white line) intensity, as no corresponding shift is observed at the L2 edge. A hydrogen-related L2,3 XANES feature at 9 eV appears with nearly equal intensity at each edge. This peak is assigned to electronic transitions from Pt 2p levels to H 1s−Pt 5d antibonding states with mixed d3/2−d5/2 character. From the L2,3 XANES analysis, we find that the number of unoccupied d states in hydrogen-covered Pt clusters is 23% less than in bulk Pt. In contrast, the L2,3 XANES spectra of bare silica-supported Pt clusters are closely similar to those of bulk Pt; quantitative analysis reveals only a slight (4%) decrease in the number of unoccupied d states.</abstract><pub>American Chemical Society</pub><doi>10.1021/jp970244e</doi><tpages>6</tpages></addata></record> |
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| source | American Chemical Society:Jisc Collections:American Chemical Society Read & Publish Agreement 2022-2024 (Reading list) |
| title | Hydrogen Chemisorption on Silica-Supported Pt Clusters: In Situ X-ray Absorption Spectroscopy |
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