Selective Activation of Methane on Single-Atom Catalyst of Rhodium Dispersed on Zirconia for Direct Conversion.
Direct methane conversion into value-added products has become increasingly important. Because of inertness of methane, cleaving the first C-H bond has been very difficult, requiring high reaction temperature on the heterogeneous catalysts. Once the first C-H bond becomes activated, the remaining C-...
| Publicado en: | Journal of the American Chemical Society Vol. 139; no. 48; pp. 17694 - 17700 |
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| Autores principales: | , , , , |
| Formato: | Artículo |
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American Chemical Society
12/6/2017
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| 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=126761846&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 126761846 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: 12/6/2017 vid: 139 iid: 48 pid: 997 pub: American Chemical Society artinfo: ui: 126761846 10.1021/jacs.7b11010 ppf: 17694 ppct: 6 formats: tig: atl: Selective Activation of Methane on Single-Atom Catalyst of Rhodium Dispersed on Zirconia for Direct Conversion. aug: au: Yongwoo Kwon Tae Yong Kim Gihun Kwon Jongheop Yi Hyunjoo Lee affil: Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology, Daejeon 34141, Republic of Korea School of Chemical and Biological Engineering, Seoul National University, Seoul 08826, Republic of Korea su: Heterogeneous catalysts synthesis Methane synthesis Rhodium Zirconium oxide Density functional theory sug: subj: Heterogeneous catalysts synthesis Methane synthesis Rhodium Zirconium oxide Density functional theory ab: Direct methane conversion into value-added products has become increasingly important. Because of inertness of methane, cleaving the first C-H bond has been very difficult, requiring high reaction temperature on the heterogeneous catalysts. Once the first C-H bond becomes activated, the remaining C-H bonds are successively dissociated on the metal surface, hindering the direct methane conversion into chemicals. Here, a single-atom Rh catalyst dispersed on ZrO surface has been synthesized and used for selective activation of methane. The Rh single atomic nature was confirmed by extended X-ray fine structure analysis, electron microscopy images, and diffuse reflectance infrared Fourier transform spectroscopy. A model of the singleatom Rh/ZrO catalyst was constructed by density functional theory calculations, and it was shown that CH intermediates can be energetically stabilized on the single-atom catalyst. The direct conversion of methane was performed using HO in the aqueous solution or using O in gas phase as oxidants. Whereas Rh nanoparticles produced CO only, the single-atom Rh catalyst produced methanol in aqueous phase or ethane in gas phase. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2017 holdings: @attributes: islocal: N |
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