Infrared Study of the Dynamics of Adsorbed Species During Co Hydrogenation
The dynamics of adsorbed species on Rh/SiO 2 catalyst during CO hydrogenation to form methane was studied using in situ infrared (IR) spectroscopy combined with steady-state isotopic transient and pulsing CO methods. In situ IR spectra and transient responses reveal that gaseous CO rapidly exchanges...
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| Veröffentlicht in: | Journal of catalysis 1995-11, Vol.157 (1), p.51-65 |
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| container_end_page | 65 |
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| container_issue | 1 |
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| container_title | Journal of catalysis |
| container_volume | 157 |
| creator | Balakos, M.W. Chuang, S.S.C. Srinivas, G. Brundage, M.A. |
| description | The dynamics of adsorbed species on Rh/SiO
2 catalyst during CO hydrogenation to form methane was studied using
in situ infrared (IR) spectroscopy combined with steady-state isotopic transient and pulsing CO methods.
In situ IR spectra and transient responses reveal that gaseous CO rapidly exchanges with adsorbed CO and hydrogenation of CH
x
intermediate is the rate-determining step under steady-state conditions. Compartment modeling and site distribution analysis of the transient responses show that CH
x
is hydrogenated to CH
4 with a bimodal distribution of the rate constant. When CO is pulsed into H
2 flow, CO dissociation is the rate-determining step and linear CO depletes faster than bridged CO. The rate-determining step for methanation is a delicate balance of intermediate concentrations, surface intrinsic properties, and reaction conditions. Mechanistic and kinetic studies of catalytic reactions have to be performed under practical reactor conditions. |
| doi_str_mv | 10.1006/jcat.1995.1267 |
| format | Article |
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2 catalyst during CO hydrogenation to form methane was studied using
in situ infrared (IR) spectroscopy combined with steady-state isotopic transient and pulsing CO methods.
In situ IR spectra and transient responses reveal that gaseous CO rapidly exchanges with adsorbed CO and hydrogenation of CH
x
intermediate is the rate-determining step under steady-state conditions. Compartment modeling and site distribution analysis of the transient responses show that CH
x
is hydrogenated to CH
4 with a bimodal distribution of the rate constant. When CO is pulsed into H
2 flow, CO dissociation is the rate-determining step and linear CO depletes faster than bridged CO. The rate-determining step for methanation is a delicate balance of intermediate concentrations, surface intrinsic properties, and reaction conditions. Mechanistic and kinetic studies of catalytic reactions have to be performed under practical reactor conditions.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1006/jcat.1995.1267</identifier><identifier>CODEN: JCTLA5</identifier><language>eng</language><publisher>Amsterdam: Elsevier Inc</publisher><subject>Catalysis ; Catalytic reactions ; Chemistry ; Exact sciences and technology ; General and physical chemistry ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><ispartof>Journal of catalysis, 1995-11, Vol.157 (1), p.51-65</ispartof><rights>1995 Academic Press</rights><rights>1995 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c381t-6710fba3aca11e2d0e0fb75a4d212496647f2358e3439807fbaf1efba8fd6ff3</citedby></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1006/jcat.1995.1267$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,777,781,3537,27905,27906,45976</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=3700655$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Balakos, M.W.</creatorcontrib><creatorcontrib>Chuang, S.S.C.</creatorcontrib><creatorcontrib>Srinivas, G.</creatorcontrib><creatorcontrib>Brundage, M.A.</creatorcontrib><title>Infrared Study of the Dynamics of Adsorbed Species During Co Hydrogenation</title><title>Journal of catalysis</title><description>The dynamics of adsorbed species on Rh/SiO
2 catalyst during CO hydrogenation to form methane was studied using
in situ infrared (IR) spectroscopy combined with steady-state isotopic transient and pulsing CO methods.
In situ IR spectra and transient responses reveal that gaseous CO rapidly exchanges with adsorbed CO and hydrogenation of CH
x
intermediate is the rate-determining step under steady-state conditions. Compartment modeling and site distribution analysis of the transient responses show that CH
x
is hydrogenated to CH
4 with a bimodal distribution of the rate constant. When CO is pulsed into H
2 flow, CO dissociation is the rate-determining step and linear CO depletes faster than bridged CO. The rate-determining step for methanation is a delicate balance of intermediate concentrations, surface intrinsic properties, and reaction conditions. Mechanistic and kinetic studies of catalytic reactions have to be performed under practical reactor conditions.</description><subject>Catalysis</subject><subject>Catalytic reactions</subject><subject>Chemistry</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><issn>0021-9517</issn><issn>1090-2694</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>1995</creationdate><recordtype>article</recordtype><recordid>eNp1kDFPwzAQhS0EEqWwMmdgTfDFcRyPVQu0qBID3S3XPhdXbVLZKVL-PY6K2FjudNJ7d_c-Qh6BFkBp_bw3ui9ASl5AWYsrMgEqaV7WsromE0pLyCUHcUvuYtxTCsB5MyHvq9YFHdBmn_3ZDlnnsv4Ls8XQ6qM3cZxnNnZhOypOaDzGbHEOvt1l8y5bDjZ0O2x177v2ntw4fYj48NunZPP6spkv8_XH22o-W-eGNdDntQDqtpppowGwtBTTKLiubAllJeu6Eq5kvEFWMdlQkbQOMNXG2do5NiXFZa0JXYwBnToFf9RhUEDVCEKNINQIQo0gkuHpYjjpaPQhxW2Nj38uJpKH8yRrLjJMv397DCqmtK1B6wOaXtnO_3fhBxcDcbU</recordid><startdate>19951101</startdate><enddate>19951101</enddate><creator>Balakos, M.W.</creator><creator>Chuang, S.S.C.</creator><creator>Srinivas, G.</creator><creator>Brundage, M.A.</creator><general>Elsevier Inc</general><general>Elsevier</general><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>19951101</creationdate><title>Infrared Study of the Dynamics of Adsorbed Species During Co Hydrogenation</title><author>Balakos, M.W. ; Chuang, S.S.C. ; Srinivas, G. ; Brundage, M.A.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c381t-6710fba3aca11e2d0e0fb75a4d212496647f2358e3439807fbaf1efba8fd6ff3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>1995</creationdate><topic>Catalysis</topic><topic>Catalytic reactions</topic><topic>Chemistry</topic><topic>Exact sciences and technology</topic><topic>General and physical chemistry</topic><topic>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Balakos, M.W.</creatorcontrib><creatorcontrib>Chuang, S.S.C.</creatorcontrib><creatorcontrib>Srinivas, G.</creatorcontrib><creatorcontrib>Brundage, M.A.</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>Balakos, M.W.</au><au>Chuang, S.S.C.</au><au>Srinivas, G.</au><au>Brundage, M.A.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Infrared Study of the Dynamics of Adsorbed Species During Co Hydrogenation</atitle><jtitle>Journal of catalysis</jtitle><date>1995-11-01</date><risdate>1995</risdate><volume>157</volume><issue>1</issue><spage>51</spage><epage>65</epage><pages>51-65</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><coden>JCTLA5</coden><abstract>The dynamics of adsorbed species on Rh/SiO
2 catalyst during CO hydrogenation to form methane was studied using
in situ infrared (IR) spectroscopy combined with steady-state isotopic transient and pulsing CO methods.
In situ IR spectra and transient responses reveal that gaseous CO rapidly exchanges with adsorbed CO and hydrogenation of CH
x
intermediate is the rate-determining step under steady-state conditions. Compartment modeling and site distribution analysis of the transient responses show that CH
x
is hydrogenated to CH
4 with a bimodal distribution of the rate constant. When CO is pulsed into H
2 flow, CO dissociation is the rate-determining step and linear CO depletes faster than bridged CO. The rate-determining step for methanation is a delicate balance of intermediate concentrations, surface intrinsic properties, and reaction conditions. Mechanistic and kinetic studies of catalytic reactions have to be performed under practical reactor conditions.</abstract><cop>Amsterdam</cop><pub>Elsevier Inc</pub><doi>10.1006/jcat.1995.1267</doi><tpages>15</tpages></addata></record> |
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| language | eng |
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| source | Elsevier ScienceDirect Journals |
| subjects | Catalysis Catalytic reactions Chemistry Exact sciences and technology General and physical chemistry Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry |
| title | Infrared Study of the Dynamics of Adsorbed Species During Co Hydrogenation |
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