File Download

There are no files associated with this item.

  Links for fulltext
     (May Require Subscription)
Supplementary

Article: A Reaction Mechanism of Methane Coupling on a Silica-Supported Single-Site Tantalum Catalyst

TitleA Reaction Mechanism of Methane Coupling on a Silica-Supported Single-Site Tantalum Catalyst
Authors
Issue Date2014
Citation
Organometallics, 2014, v. 33, p. 2172-2181 How to Cite?
AbstractDensity functional theory calculations were utilized to study the reaction mechanisms of nonoxidative coupling of methane (NOCM) occurring on a silica-supported single-site tantalum (Ta) catalyst. Two catalytic cycles, namely, catalytic cycles A (CCA) and B (CCB), as well as other competing pathways, were investigated by exploring the potential energy surfaces for the reactions of interest. The supported methyltantalum [(≡SiO3)2Ta–CH3] and tantalum hydride [(≡SiO3)2Ta–H] catalyzed the reaction of NOCM through CCA and CCB, respectively. CCA and CCB comprise five and six elementary steps, respectively. The two rate-determining states for both catalytic cycles were elucidated. The turnover number of methane conversion catalyzed by the supported methyltantalum was about 105 larger than that catalyzed by the supported tantalum hydride. This large difference indicates that the former species is predominantly responsible for the conversion of methane to ethane.
Persistent Identifierhttp://hdl.handle.net/10722/202575
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorLin, Xen_US
dc.contributor.authorXi, Yen_US
dc.contributor.authorZhang, Gen_US
dc.contributor.authorPhillips, DLen_US
dc.contributor.authorGuo, Wen_US
dc.date.accessioned2014-09-19T08:41:24Z-
dc.date.available2014-09-19T08:41:24Z-
dc.date.issued2014en_US
dc.identifier.citationOrganometallics, 2014, v. 33, p. 2172-2181en_US
dc.identifier.urihttp://hdl.handle.net/10722/202575-
dc.description.abstractDensity functional theory calculations were utilized to study the reaction mechanisms of nonoxidative coupling of methane (NOCM) occurring on a silica-supported single-site tantalum (Ta) catalyst. Two catalytic cycles, namely, catalytic cycles A (CCA) and B (CCB), as well as other competing pathways, were investigated by exploring the potential energy surfaces for the reactions of interest. The supported methyltantalum [(≡SiO3)2Ta–CH3] and tantalum hydride [(≡SiO3)2Ta–H] catalyzed the reaction of NOCM through CCA and CCB, respectively. CCA and CCB comprise five and six elementary steps, respectively. The two rate-determining states for both catalytic cycles were elucidated. The turnover number of methane conversion catalyzed by the supported methyltantalum was about 105 larger than that catalyzed by the supported tantalum hydride. This large difference indicates that the former species is predominantly responsible for the conversion of methane to ethane.en_US
dc.languageengen_US
dc.relation.ispartofOrganometallicsen_US
dc.titleA Reaction Mechanism of Methane Coupling on a Silica-Supported Single-Site Tantalum Catalysten_US
dc.typeArticleen_US
dc.identifier.emailPhillips, DL: phillips@hku.hken_US
dc.identifier.authorityPhillips, DL=rp00770en_US
dc.identifier.doi10.1021/om400996fen_US
dc.identifier.hkuros237044en_US
dc.identifier.volume33en_US
dc.identifier.spage2172en_US
dc.identifier.epage2181en_US
dc.identifier.isiWOS:000335939900008-

Export via OAI-PMH Interface in XML Formats


OR


Export to Other Non-XML Formats