Photo-CIDNP Reveals Different Protonation Sites Depending on the Primary Step of the Photoinduced Electron-/Proton-Transfer Process with Ru(II) Polyazaaromatic Complexes.
The excited-state quenching of [Ru- (TAP)(HAT)] (TAP = 1,4,5,8-tetraazaphenanthrene, HAT= 1,4,5,8,9,12-hexaazatriphenylene) by hydroquinone (H2Q), N-acetyl-tyrosine (N-Ac-Tyr) or guanosine-5'- monophosphate (GMP) was investigated at various pH values. The quenching occurs via electron/proton transfe...
| Publicado en: | Journal of the American Chemical Society Vol. 139; no. 42; pp. 14909 - 14913 |
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| Autores principales: | , , , , , |
| Formato: | Artículo |
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American Chemical Society
10/25/2017
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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=125899047&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 125899047 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: 10/25/2017 vid: 139 iid: 42 pid: 997 pub: American Chemical Society artinfo: ui: 125899047 10.1021/jacs.7b09513 ppf: 14909 ppct: 4 formats: tig: atl: Photo-CIDNP Reveals Different Protonation Sites Depending on the Primary Step of the Photoinduced Electron-/Proton-Transfer Process with Ru(II) Polyazaaromatic Complexes. aug: au: Troian-Gautier, Ludovic Mugeniwabagara, Epiphanie Fusaro, Luca Cauët, Emilie Kirsch-De Mesmaeker, Andrée Luhmer, Michel affil: Laboratoire de Chimie Organique et Photochimie (CP 160/08) Department of Chemistry, Murray Hall, University of North Carolina at Chapel Hill, 123 South Road, Chapel Hill, North Carolina 25799, United States Laboratoire de Résonance Magnétique Nucléaire Haute Résolution (CP 160/08) Chimie des Nanomateériaux (CNANO), Universitéde Namur, 61 rue de Bruxelles B-5000 Namur, Belgium Service de Chimie Quantique et Photophysique (CP 160/09), Universiteélibre de Bruxelles, 50 av. F. D. Roosevelt, B-1050 Brussels, Belgium su: Proton transfer reactions Hydroquinone Polarization (Nuclear physics) Density functional theory Charge exchange sug: subj: Proton transfer reactions Hydroquinone Polarization (Nuclear physics) Density functional theory Charge exchange ab: The excited-state quenching of [Ru- (TAP)(HAT)] (TAP = 1,4,5,8-tetraazaphenanthrene, HAT= 1,4,5,8,9,12-hexaazatriphenylene) by hydroquinone (H2Q), N-acetyl-tyrosine (N-Ac-Tyr) or guanosine-5'- monophosphate (GMP) was investigated at various pH values. The quenching occurs via electron/proton transfer, as evidenced by transient absorption spectroscopy and confirmed by H photochemically induced dynamic nuclear polarization (photo-CIDNP). Reductive quenching also occurs in strongly acidic solution despite a much shorter lifetime of the protonated excited-state complex. Photo-CIDNP revealed a different mechanism at low pH, involving protonation before electron transfer and yielding a distinct protonated monoreduced complex. The experimental photo-CIDNP patterns are consistent with density functional theory calculations. This work highlights the power of 1H photo-CIDNP for characterizing, at the atomic level, transient species involved in electron-transfer processes. 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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