Solution Structures of Highly Active Molecular Ir Water-Oxidation Catalysts from Density Functional Theory Combined with High- Energy X-ray Scattering and EXAFS Spectroscopy.
The solution structures of highly active Ir water-oxidation catalysts are elucidated by combining density functional theory, high-energy X-ray scattering (HEXS), and extended X-ray absorption fine structure (EXAFS) spectroscopy. We find that the catalysts are Ir dimers with mono-p-O cores and termin...
| Publicado en: | Journal of the American Chemical Society Vol. 138; no. 17; pp. 5511 - 5515 |
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| Autores principales: | , , , , , , , , , , |
| Formato: | Artículo |
| Publicado: |
American Chemical Society
5/4/2016
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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=115656366&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 115656366 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: 5/4/2016 vid: 138 iid: 17 pid: 997 pub: American Chemical Society artinfo: ui: 115656366 10.1021/jacs.6b01750 ppf: 5511 ppct: 4 formats: tig: atl: Solution Structures of Highly Active Molecular Ir Water-Oxidation Catalysts from Density Functional Theory Combined with High- Energy X-ray Scattering and EXAFS Spectroscopy. aug: au: Yang, Ke R. Matula, Adam J. Gihan Kwon Jiyun Hong Sheehan, Stafford W. Thomsen, Julianne M. Brudvig, Gary W. Crabtree, Robert H. Tiede, David M. Chen, Lin X. Batista, Victor S. affil: Yale Energy Sciences Institute and Department of Chemistry, Yale University, New Haven, Connecticut 06520-8107, United States Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, Illinois 60439, United States Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States Catalytic Innovations LLC, 70 Crandall Road, PO Box 356, Adamsville, Rhode Island, 02801, United States su: Oxidation of water Iridium catalysts Density functional theory X-ray scattering Extended X-ray absorption fine structure Partial oxidation sug: subj: Oxidation of water Iridium catalysts Density functional theory X-ray scattering Extended X-ray absorption fine structure Partial oxidation ab: The solution structures of highly active Ir water-oxidation catalysts are elucidated by combining density functional theory, high-energy X-ray scattering (HEXS), and extended X-ray absorption fine structure (EXAFS) spectroscopy. We find that the catalysts are Ir dimers with mono-p-O cores and terminal anionic ligands, generated in situ through partial oxidation of a common catalyst precursor. The proposed structures are supported by H and O NMR, EPR, resonance Raman and UV-vis spectra, electrophoresis, etc. Our findings are particularly valuable to understand the mechanism of water oxidation by highly reactive Ir catalysts. Importantly, our DFTEXAFS- HEXS methodology provides a new in situ technique for characterization of active species in catalytic systems. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2016 holdings: @attributes: islocal: N |
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