Journal ArticleDOI
Excited-state quenching by proton-coupled electron transfer
Javier J. Concepcion,M. Kyle Brennaman,Jeremy R. Deyton,Natalia V. Lebedeva,Malcolm D. E. Forbes,John M. Papanikolas,Thomas J. Meyer +6 more
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TLDR
The protonated, reduced complex [Ru(bpy)2(bpzH•)]2+ functions as a H-atom reductant toward quinone or benzaldehyde with potential implications for net photochemistry and energy conversion.Abstract:
The emitting metal-to-ligand charge transfer (MLCT) excited state of [Ru(bpy)2(bpz)]2+ (bpy is 2,2‘-bipyridine; bpz is 2,2‘-bipyrazine) is reductively quenched by hydroquinone (H2Q) by proton-coupled electron transfer (PCET), most likely by concerted electron−proton transfer (EPT). The identity of the transient products ([Ru(bpy)2(bpzH•)]2+ and HQ•) and the kinetics of their formation and disappearance have been established by steady-state emission and time-resolved emission, absorption, and EPR measurements. The protonated, reduced complex [Ru(bpy)2(bpzH•)]2+ functions as a H-atom reductant toward quinone or benzaldehyde with potential implications for net photochemistry and energy conversion.read more
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Impacts of the Location and Number of [Cu(bpy)2]2+ Cross-Links on the Emission Photodynamics of [Ru(bpy)3]2+ with Pendant Oligo(aminoethylglycine) Chains
TL;DR: It is demonstrated that metal coordination self-assembles structures made from modular artificial amino acids can provide controlled arrangements of chromophores, electron donors, and electron acceptors to shuttle electrons in a new approach for mimicking photosynthesis.
Journal ArticleDOI
FRET sensitization of tungsten-alkylidyne complexes by zinc porphyrins in self-assembled dyads.
TL;DR: The mechanism and rates of the net S(1)→(3)[dπ*] energy transfer are found to differ significantly from those for previously reported zinc-porphyrin/tungsten-alkylidyne dyads that are constructed from similar components but connected instead with covalent bonds at the porphyrin edge.
Journal ArticleDOI
Competing Pathways in the photo-Proton-Coupled Electron Transfer Reduction of fac-[Re(bpy)(CO)3(4,4′-bpy]+* by Hydroquinone
David J. Stewart,M. Kyle Brennaman,Stephanie E. Bettis,Li Wang,Robert A. Binstead,John M. Papanikolas,Thomas J. Meyer +6 more
TL;DR: In this article, the metal-to-ligand charge transfer (MLCT) excited state of fac-[ReI(bpy)(CO)3(4,4′-bpy)]+ is reductively quenched by 1,4-hydroquinone (H2Q) in CH3CN at 23 ± 2 °C by competing pathways to give a common electronproton-transfer intermediate.
Journal ArticleDOI
Visible light water disinfection using [Ru(bpy)2(phendione)](PF6)2·2H2O and [Ru(phendione)3]Cl2·2H2O complexes and their effective adsorption onto activated carbon
TL;DR: In this article, Ru(II) polypyridyl complexes [Ru(bpy)2(phendione)](PF6)2·2H2O (complex1) and [Ru[Phendione)3]Cl2·1.5,5,6-dione (complex2) showed complete photoinactivation of Gram positive and negative bacteria on photolysis using light emitting diode array as visible light source.
Journal ArticleDOI
Photo-triggered hydrogen atom transfer from an iridium hydride complex to unactivated olefins
TL;DR: The photo-HAT reactivity presented here represents a conceptually novel approach to photocatalysis with metal complexes, which is fundamentally different from the many prior studies relying on photoinduced electron transfer.
References
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Journal ArticleDOI
Water-splitting chemistry of photosystem II.
James P. McEvoy,Gary W. Brudvig +1 more
TL;DR: Life on earth is almost entirely solar-powered, with carbohydrate acting as a source of high-energy electrons and dioxygen providing a lower-energy destination for these electrons.
Journal ArticleDOI
Chemical approaches to artificial photosynthesis. 2.
TL;DR: The underlying physical principles--light absorption, energy transfer, radiative and nonradiative excited-state decay, electron transfer, proton-coupled electronTransfer, and catalysis--are outlined with an eye toward their roles in molecular assemblies for energy conversion.
Journal ArticleDOI
Proton-coupled electron transfer: a reaction chemist's view.
TL;DR: Intrinsic barriers for PCET can be comparable to or larger than those for ET, and many PCET/HAT rate constants are predicted well by the Marcus cross relation.
Journal ArticleDOI
Theoretical Perspectives on Proton-Coupled Electron Transfer Reactions
TL;DR: This theoretical framework allows predictions of rates, mechanisms, and kinetic isotope effects for proton-coupled electron transfer reactions.
Journal ArticleDOI
Oxygen Production in Nature: A Light-Driven Metalloradical Enzyme Process
Cecilia Tommos,Gerald T. Babcock +1 more
TL;DR: The physical structure and energetics of PSII are reviewed and a metalloradical enzyme mechanism for the water-oxidation process it catalyzes is discussed, which is based on the specifics of the chemistry in which O2 participates.