title: Photoproduction of Hydrogen by Decamethylruthenocene Combined with Electrochemical Recycling.
abstract: The photoinduced hydrogen evolution reaction (HER) by decamethylruthenocene, Cp2*RuII(Cp*=C5Me5), is reported. The use of a metallocene to photoproduce hydrogen is presented as an alternative strategy to reduce protons without involving an additional photosensitizer. The mechanism was investigated by (spectro)electrochemical and spectroscopic (UV/Vis and1H NMR) measurements. The photoactivated hydride involved was characterized spectroscopically and the resulting [Cp2*RuIII]+species was electrochemically regenerated in situ on a fluorinated tin oxide electrode surface. A promising internal quantum yield of 25 % was obtained. Optimal experimental conditions- especially the use of weakly coordinating solvent and counterions-are discussed.
authors.affiliation: Laboratoire d'Electrochimie Physique et Analytique (LEPA), École Polytechnique Fédérale de Lausanne (EPFL Valais Wallis), Rue de l'Industrie, 17, 1951, Sion, Switzerland.
authors.forename: Lucie
authors.initials: L
authors.lastname: Rivier
authors.affiliation: Laboratoire d'Electrochimie Physique et Analytique (LEPA), École Polytechnique Fédérale de Lausanne (EPFL Valais Wallis), Rue de l'Industrie, 17, 1951, Sion, Switzerland.
authors.forename: Pekka
authors.identifier: 0000-0002-1229-2261
authors.initials: P
authors.lastname: Peljo
authors.affiliation: Laboratory for Computational Molecular Design, École Polytechnique Fédérale de Lausanne (EPFL), Route Cantonal, 33, 1015, Lausanne, Switzerland.
authors.forename: Laurent A C
authors.initials: LA
authors.lastname: Vannay
authors.affiliation: Laboratoire d'Electrochimie Physique et Analytique (LEPA), École Polytechnique Fédérale de Lausanne (EPFL Valais Wallis), Rue de l'Industrie, 17, 1951, Sion, Switzerland.
authors.forename: Grégoire C
authors.initials: GC
authors.lastname: Gschwend
authors.affiliation: Laboratoire d'Electrochimie Physique et Analytique (LEPA), École Polytechnique Fédérale de Lausanne (EPFL Valais Wallis), Rue de l'Industrie, 17, 1951, Sion, Switzerland.
authors.forename: Manuel A
authors.initials: MA
authors.lastname: Méndez
authors.affiliation: Laboratory for Computational Molecular Design, École Polytechnique Fédérale de Lausanne (EPFL), Route Cantonal, 33, 1015, Lausanne, Switzerland.
authors.forename: Clémence
authors.identifier: 0000-0001-7993-2879
authors.initials: C
authors.lastname: Corminboeuf
authors.affiliation: Department of Chemistry, the Tyndall National Institute and the Analytical and Biological Research Facility (ABCRF), University College Cork, Cork, Ireland.
authors.forename: Micheál D
authors.identifier: 0000-0001-7951-7085
authors.initials: MD
authors.lastname: Scanlon
authors.affiliation: Laboratoire d'Electrochimie Physique et Analytique (LEPA), École Polytechnique Fédérale de Lausanne (EPFL Valais Wallis), Rue de l'Industrie, 17, 1951, Sion, Switzerland.
authors.forename: Hubert H
authors.identifier: 0000-0001-5573-5774
authors.initials: HH
authors.lastname: Girault
keywords: decamethylruthenocene; electrocatalysis; hydrogen evolution reaction; metallocenes