Direct Conversion of Methane to Methanol on Ni-Ceria Surfaces: Metal-Support Interactions and Water-Enabled Catalytic Conversion by Site Blocking.
The transformation of methane into methanol or higher alcohols at moderate temperature and pressure conditions is of great environmental interest and remains a challenge despite many efforts. Extended surfaces of metallic nickel are inactive for a direct CH → CHOH conversion. This experimental and c...
| Publicado en: | Journal of the American Chemical Society Vol. 140; no. 24; pp. 7681 - 7688 |
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| Autores principales: | , , , , , , , , , , |
| Formato: | Artículo |
| Publicado: |
American Chemical Society
6/20/2018
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| Materias: | |
| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=130322047&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 130322047 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 6/20/2018 vid: 140 iid: 24 pid: 997 pub: American Chemical Society artinfo: ui: 130322047 10.1021/jacs.8b03809 ppf: 7681 ppct: 7 formats: tig: atl: Direct Conversion of Methane to Methanol on Ni-Ceria Surfaces: Metal-Support Interactions and Water-Enabled Catalytic Conversion by Site Blocking. aug: au: Lustemberg, Pablo G. Palomino, Robert M. Gutie'rrez, Ramo'n A. Grinter, David C. Vorokhta, Mykhailo Zongyuan Liu Ramírez, Pedro J. Matolín, Vladimír Ganduglia-Pirovano, M. Vero'nica Senanayake, Sanjaya D. Rodriguez, Jose' A. affil: Instituto de Fisica Rosario (IFIR), CONICET-UNR, Bv. 27 de Febrero 210bis, S2000EZP Rosario, Santa Fe, Argentina Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973, United States Facultad de Ciencias, Universidad Central de Venezuela, Caracas 1020-A, Venezuela Surfaces and Interfaces, Diamond Light Source, Harwell Science and Innovation Campus, Didcot, Oxfordshire OX11 0DE, United Kingdom Department of Surface and Plasma Science, Faculty of Mathematics and Physics, Charles University, Prague, Czech Republic Instituto de Cata'lisis y Petroleoquímica, CSIC, C/Marie Curie 2, 28049 Madrid, Spain su: Methane Methanol Density functional theory Nickel Metal catalysts sug: subj: Methane Methanol Density functional theory Nickel Metal catalysts ab: The transformation of methane into methanol or higher alcohols at moderate temperature and pressure conditions is of great environmental interest and remains a challenge despite many efforts. Extended surfaces of metallic nickel are inactive for a direct CH → CHOH conversion. This experimental and computational study provides clear evidence that low Ni loadings on a CeO(111) support can perform a direct catalytic cycle for the generation of methanol at low temperature using oxygen and water as reactants, with a higher selectivity than ever reported for ceria-based catalysts. On the basis of ambient pressure X-ray photoemission spectroscopy and density functional theory calculations, we demonstrate that water plays a crucial role in blocking catalyst sites where methyl species could fully decompose, an essential factor for diminishing the production of CO and CO, and in generating sites on which methoxy species and ultimately methanol can form. In addition to water-site blocking, one needs the effects of metal-support interactions to bind and activate methane and water. These findings should be considered when designing metal/oxide catalysts for converting methane to value-added chemicals and fuels. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2018 holdings: @attributes: islocal: N |
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