Influence of support ionicity on the hydrogen chemisorption of Pt particles dispersed in Y zeolite: consequences for Pt particle size determination using the H/M method
Zeolite Y-supported Pt particles were studied by high-resolution transmission electron microscopy (HRTEM), extended X-ray absorption fine structure (EXAFS), and H 2 chemisorption experiments. The ionicity (i.e., electron richness of the zeolite oxygen atoms) was altered by using different cations (N...
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| Veröffentlicht in: | Journal of catalysis 2005-09, Vol.234 (2), p.376-384 |
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| creator | Ji, Yaying van der Eerden, Ad M.J. Koot, Vincent Kooyman, Patricia J. Meeldijk, Johannes D. Weckhuysen, Bert M. Koningsberger, Diek C. |
| description | Zeolite Y-supported Pt particles were studied by high-resolution transmission electron microscopy (HRTEM), extended X-ray absorption fine structure (EXAFS), and H
2 chemisorption experiments. The ionicity (i.e., electron richness of the zeolite oxygen atoms) was altered by using different cations (NaY, MgY, and LaY) and by steaming and introduction of protons (H-USY). Highly dispersed Pt particles were introduced inside the zeolite pores using a very careful synthesis procedure. Computer analysis of HRTEM images exhibited similar Pt particle size distributions with calculated average Pt particle sizes ranging from 0.98 to 1.26 nm for the various zeolite Y-supported Pt particles. The EXAFS results revealed that the first-shell Pt–Pt coordination number was around 6.5, in good agreement with the observed HRTEM results. H
2 chemisorption experiments found a much higher H/Pt value for Pt/NaY (1.63) than for Pt/H-USY(0.88), implying no relationship with the Pt dispersion as determined by HRTEM. Using the values for the dispersion (Pt
s/Pt) as calculated from the HRTEM results, one can obtain a value for the number of chemisorbed hydrogen atoms per surface platinum atom (H/Pt
s ratio). This value demonstrates a clearly decreasing trend with decreasing electron richness of the support oxygen atom: 1.96 (Pt/NaY)
>
1.74 (Pt/MgY)
>
1.51 (Pt/LaY)
>
1.11 (Pt/H-USY). These results indicate that the hydrogen coverage on supported Pt particles depends strongly on the support ionicity. This has significant consequences for the catalytic behavior of hydrogenolysis and hydrogenation reactions catalyzed by Pt. These results also indicate that one should be cautious in interpreting H
2 chemisorption results only in terms of Pt dispersion. This approach is valid only when comparing Pt particles dispersed on the same support. Serious deviations in the real Pt dispersions occur if Pt is supported on oxides with different ionicities. |
| doi_str_mv | 10.1016/j.jcat.2005.06.030 |
| format | Article |
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2 chemisorption experiments. The ionicity (i.e., electron richness of the zeolite oxygen atoms) was altered by using different cations (NaY, MgY, and LaY) and by steaming and introduction of protons (H-USY). Highly dispersed Pt particles were introduced inside the zeolite pores using a very careful synthesis procedure. Computer analysis of HRTEM images exhibited similar Pt particle size distributions with calculated average Pt particle sizes ranging from 0.98 to 1.26 nm for the various zeolite Y-supported Pt particles. The EXAFS results revealed that the first-shell Pt–Pt coordination number was around 6.5, in good agreement with the observed HRTEM results. H
2 chemisorption experiments found a much higher H/Pt value for Pt/NaY (1.63) than for Pt/H-USY(0.88), implying no relationship with the Pt dispersion as determined by HRTEM. Using the values for the dispersion (Pt
s/Pt) as calculated from the HRTEM results, one can obtain a value for the number of chemisorbed hydrogen atoms per surface platinum atom (H/Pt
s ratio). This value demonstrates a clearly decreasing trend with decreasing electron richness of the support oxygen atom: 1.96 (Pt/NaY)
>
1.74 (Pt/MgY)
>
1.51 (Pt/LaY)
>
1.11 (Pt/H-USY). These results indicate that the hydrogen coverage on supported Pt particles depends strongly on the support ionicity. This has significant consequences for the catalytic behavior of hydrogenolysis and hydrogenation reactions catalyzed by Pt. These results also indicate that one should be cautious in interpreting H
2 chemisorption results only in terms of Pt dispersion. This approach is valid only when comparing Pt particles dispersed on the same support. Serious deviations in the real Pt dispersions occur if Pt is supported on oxides with different ionicities.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/j.jcat.2005.06.030</identifier><identifier>CODEN: JCTLA5</identifier><language>eng</language><publisher>Amsterdam: Elsevier Inc</publisher><subject>Catalysis ; Chemistry ; Exact sciences and technology ; General and physical chemistry ; H/M method ; High-resolution transmission electron microscopy ; Hydrogen chemisorption ; Ion-exchange ; Metal–support interaction ; Particle size determination ; Support ionicity ; Surface physical chemistry ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry ; Zeolites: preparations and properties</subject><ispartof>Journal of catalysis, 2005-09, Vol.234 (2), p.376-384</ispartof><rights>2005 Elsevier Inc.</rights><rights>2005 INIST-CNRS</rights><rights>Copyright © 2005 Elsevier B.V. All rights reserved.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c467t-f7c9af4e9ecfff46415479886a252da9fb35d81f9233ac26fb9a728343cbeb6e3</citedby></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.jcat.2005.06.030$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,780,784,3550,27924,27925,45995</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=17067411$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Ji, Yaying</creatorcontrib><creatorcontrib>van der Eerden, Ad M.J.</creatorcontrib><creatorcontrib>Koot, Vincent</creatorcontrib><creatorcontrib>Kooyman, Patricia J.</creatorcontrib><creatorcontrib>Meeldijk, Johannes D.</creatorcontrib><creatorcontrib>Weckhuysen, Bert M.</creatorcontrib><creatorcontrib>Koningsberger, Diek C.</creatorcontrib><title>Influence of support ionicity on the hydrogen chemisorption of Pt particles dispersed in Y zeolite: consequences for Pt particle size determination using the H/M method</title><title>Journal of catalysis</title><description>Zeolite Y-supported Pt particles were studied by high-resolution transmission electron microscopy (HRTEM), extended X-ray absorption fine structure (EXAFS), and H
2 chemisorption experiments. The ionicity (i.e., electron richness of the zeolite oxygen atoms) was altered by using different cations (NaY, MgY, and LaY) and by steaming and introduction of protons (H-USY). Highly dispersed Pt particles were introduced inside the zeolite pores using a very careful synthesis procedure. Computer analysis of HRTEM images exhibited similar Pt particle size distributions with calculated average Pt particle sizes ranging from 0.98 to 1.26 nm for the various zeolite Y-supported Pt particles. The EXAFS results revealed that the first-shell Pt–Pt coordination number was around 6.5, in good agreement with the observed HRTEM results. H
2 chemisorption experiments found a much higher H/Pt value for Pt/NaY (1.63) than for Pt/H-USY(0.88), implying no relationship with the Pt dispersion as determined by HRTEM. Using the values for the dispersion (Pt
s/Pt) as calculated from the HRTEM results, one can obtain a value for the number of chemisorbed hydrogen atoms per surface platinum atom (H/Pt
s ratio). This value demonstrates a clearly decreasing trend with decreasing electron richness of the support oxygen atom: 1.96 (Pt/NaY)
>
1.74 (Pt/MgY)
>
1.51 (Pt/LaY)
>
1.11 (Pt/H-USY). These results indicate that the hydrogen coverage on supported Pt particles depends strongly on the support ionicity. This has significant consequences for the catalytic behavior of hydrogenolysis and hydrogenation reactions catalyzed by Pt. These results also indicate that one should be cautious in interpreting H
2 chemisorption results only in terms of Pt dispersion. This approach is valid only when comparing Pt particles dispersed on the same support. Serious deviations in the real Pt dispersions occur if Pt is supported on oxides with different ionicities.</description><subject>Catalysis</subject><subject>Chemistry</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>H/M method</subject><subject>High-resolution transmission electron microscopy</subject><subject>Hydrogen chemisorption</subject><subject>Ion-exchange</subject><subject>Metal–support interaction</subject><subject>Particle size determination</subject><subject>Support ionicity</subject><subject>Surface physical chemistry</subject><subject>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><subject>Zeolites: preparations and properties</subject><issn>0021-9517</issn><issn>1090-2694</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2005</creationdate><recordtype>article</recordtype><recordid>eNp9kUFv1DAQhS0EEkvhD3CykDgmtR3HiREXVAGtVAQHOHCyvM646yhrB4-30vYX8TNJdivBidNcvvfezDxCXnNWc8bV5ViPzpZaMNbWTNWsYU_IhjPNKqG0fEo2jAle6ZZ3z8kLxJExztu235DfN9FPB4gOaPIUD_OccqEhxeBCOdIUadkB3R2HnO4gUreDfcCU57Igq-JbobPNJbgJkA4BZ8gIAw2R_qQPkKZQ4B11KSL8OqUg9Sn_q6IYHoAOUCDvQ7Qn3wOGeHcKvr78QvdQdml4SZ55OyG8epwX5Menj9-vrqvbr59vrj7cVk6qrlS-c9p6CRqc914qyVvZ6b5XVrRisNpvm3boudeiaawTym-17UTfyMZtYauguSBvzr5zTsvKWMyYDjkukYbrVspGiG6BxBlyOSFm8GbOYW_z0XBm1kLMaNZCzFqIYcoshSyit4_OFp2dfLbRBfyr7JjqJOcL9_7MwXLmfYBs0IX1d0PI4IoZUvhfzB-0xKVH</recordid><startdate>20050910</startdate><enddate>20050910</enddate><creator>Ji, Yaying</creator><creator>van der Eerden, Ad M.J.</creator><creator>Koot, Vincent</creator><creator>Kooyman, Patricia J.</creator><creator>Meeldijk, Johannes D.</creator><creator>Weckhuysen, Bert M.</creator><creator>Koningsberger, Diek C.</creator><general>Elsevier Inc</general><general>Elsevier</general><general>Elsevier BV</general><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>20050910</creationdate><title>Influence of support ionicity on the hydrogen chemisorption of Pt particles dispersed in Y zeolite: consequences for Pt particle size determination using the H/M method</title><author>Ji, Yaying ; van der Eerden, Ad M.J. ; Koot, Vincent ; Kooyman, Patricia J. ; Meeldijk, Johannes D. ; Weckhuysen, Bert M. ; Koningsberger, Diek C.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c467t-f7c9af4e9ecfff46415479886a252da9fb35d81f9233ac26fb9a728343cbeb6e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2005</creationdate><topic>Catalysis</topic><topic>Chemistry</topic><topic>Exact sciences and technology</topic><topic>General and physical chemistry</topic><topic>H/M method</topic><topic>High-resolution transmission electron microscopy</topic><topic>Hydrogen chemisorption</topic><topic>Ion-exchange</topic><topic>Metal–support interaction</topic><topic>Particle size determination</topic><topic>Support ionicity</topic><topic>Surface physical chemistry</topic><topic>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><topic>Zeolites: preparations and properties</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ji, Yaying</creatorcontrib><creatorcontrib>van der Eerden, Ad M.J.</creatorcontrib><creatorcontrib>Koot, Vincent</creatorcontrib><creatorcontrib>Kooyman, Patricia J.</creatorcontrib><creatorcontrib>Meeldijk, Johannes D.</creatorcontrib><creatorcontrib>Weckhuysen, Bert M.</creatorcontrib><creatorcontrib>Koningsberger, Diek C.</creatorcontrib><collection>Pascal-Francis</collection><collection>CrossRef</collection><jtitle>Journal of catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ji, Yaying</au><au>van der Eerden, Ad M.J.</au><au>Koot, Vincent</au><au>Kooyman, Patricia J.</au><au>Meeldijk, Johannes D.</au><au>Weckhuysen, Bert M.</au><au>Koningsberger, Diek C.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Influence of support ionicity on the hydrogen chemisorption of Pt particles dispersed in Y zeolite: consequences for Pt particle size determination using the H/M method</atitle><jtitle>Journal of catalysis</jtitle><date>2005-09-10</date><risdate>2005</risdate><volume>234</volume><issue>2</issue><spage>376</spage><epage>384</epage><pages>376-384</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><coden>JCTLA5</coden><abstract>Zeolite Y-supported Pt particles were studied by high-resolution transmission electron microscopy (HRTEM), extended X-ray absorption fine structure (EXAFS), and H
2 chemisorption experiments. The ionicity (i.e., electron richness of the zeolite oxygen atoms) was altered by using different cations (NaY, MgY, and LaY) and by steaming and introduction of protons (H-USY). Highly dispersed Pt particles were introduced inside the zeolite pores using a very careful synthesis procedure. Computer analysis of HRTEM images exhibited similar Pt particle size distributions with calculated average Pt particle sizes ranging from 0.98 to 1.26 nm for the various zeolite Y-supported Pt particles. The EXAFS results revealed that the first-shell Pt–Pt coordination number was around 6.5, in good agreement with the observed HRTEM results. H
2 chemisorption experiments found a much higher H/Pt value for Pt/NaY (1.63) than for Pt/H-USY(0.88), implying no relationship with the Pt dispersion as determined by HRTEM. Using the values for the dispersion (Pt
s/Pt) as calculated from the HRTEM results, one can obtain a value for the number of chemisorbed hydrogen atoms per surface platinum atom (H/Pt
s ratio). This value demonstrates a clearly decreasing trend with decreasing electron richness of the support oxygen atom: 1.96 (Pt/NaY)
>
1.74 (Pt/MgY)
>
1.51 (Pt/LaY)
>
1.11 (Pt/H-USY). These results indicate that the hydrogen coverage on supported Pt particles depends strongly on the support ionicity. This has significant consequences for the catalytic behavior of hydrogenolysis and hydrogenation reactions catalyzed by Pt. These results also indicate that one should be cautious in interpreting H
2 chemisorption results only in terms of Pt dispersion. This approach is valid only when comparing Pt particles dispersed on the same support. Serious deviations in the real Pt dispersions occur if Pt is supported on oxides with different ionicities.</abstract><cop>Amsterdam</cop><pub>Elsevier Inc</pub><doi>10.1016/j.jcat.2005.06.030</doi><tpages>9</tpages><oa>free_for_read</oa></addata></record> |
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| ispartof | Journal of catalysis, 2005-09, Vol.234 (2), p.376-384 |
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| subjects | Catalysis Chemistry Exact sciences and technology General and physical chemistry H/M method High-resolution transmission electron microscopy Hydrogen chemisorption Ion-exchange Metal–support interaction Particle size determination Support ionicity Surface physical chemistry Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Zeolites: preparations and properties |
| title | Influence of support ionicity on the hydrogen chemisorption of Pt particles dispersed in Y zeolite: consequences for Pt particle size determination using the H/M method |
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