First-Principles Modeling of a Dye-Sensitized TiO/lrO Photoanode for Water Oxidation.
We present a first-principle computational modeling investigation, based on density functional theory (DFT) and time-dependent DFT, on the structural, electronic, optical, and charge generation properties of the semiconductor/dye/catalyst heterointerfaces in a prototypical dye-sensitized photoanode...
| Publicado en: | Journal of the American Chemical Society Vol. 137; no. 17; pp. 5798 - 5810 |
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| Autores principales: | , |
| Formato: | Artículo |
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American Chemical Society
5/6/2015
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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=102837737&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 102837737 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: 5/6/2015 vid: 137 iid: 17 pid: 997 pub: American Chemical Society artinfo: ui: 102837737 10.1021/jacs.5b02128 ppf: 5798 ppct: 12 formats: tig: atl: First-Principles Modeling of a Dye-Sensitized TiO/lrO Photoanode for Water Oxidation. aug: au: Pastore, Mariachiara De Angelis, Filippo affil: Computational Laboratory for Hybrid Organic Photovoltaics (CLHYO), CNR-ISTM, via Elce di Sotto 8, 1-06123 Perugia, Italy su: Oxidation Anodes Density functional theory Chemical reactions Charge exchange Catalysts sug: subj: Oxidation Anodes Density functional theory Chemical reactions Charge exchange Catalysts ab: We present a first-principle computational modeling investigation, based on density functional theory (DFT) and time-dependent DFT, on the structural, electronic, optical, and charge generation properties of the semiconductor/dye/catalyst heterointerfaces in a prototypical dye-sensitized photoanode for water oxidation. The investigated architecture comprises a Ru(ll) dye-sensitized TiO substrate tethered to an IrO nanoparticle catalyst. Our realistic modeling strategy and quantitative analysis of the relevant interfacial hole/electron transfer reactions indicates the slow hole injection into IrO and the fast dye excited-state quenching to IrO as the primary sources of the relatively poor cell efficiency experimentally observed. On the basis of this atomistic and electronic structure information, we propose and computationally test, against a prototype dye, a new class of Ru(II) sensitizers, which show potentially improved photoelectrochemical performances. This study constitutes a first step toward the computer-assisted design of new and more efficient materials for solar fuels production through dye-sensitized photoelectrochemical cells. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2015 holdings: @attributes: islocal: N |
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