An efficient Ru(II) -Rh(III) -Ru(II) polypyridyl photocatalyst for visible-light-driven hydrogen production in aqueous solution

Autor: Michel Sliwa, Carmen E. Castillo, Thibaut Stoll, Fabrice Odobel, Olivier Poizat, Marie-Noëlle Collomb, Marcello Gennari, Jérôme Fortage, Alain Deronzier, Mateusz Rebarz
Přispěvatelé: Département de Chimie Moléculaire - Chimie Inorganique Redox (DCM - CIRE), Département de Chimie Moléculaire (DCM), Université Joseph Fourier - Grenoble 1 (UJF)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 (LASIRE), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Chimie Et Interdisciplinarité : Synthèse, Analyse, Modélisation (CEISAM), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie Moléculaire de Grenoble (ICMG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Département de Chimie Moléculaire - Chimie Inorganique Redox Biomimétique (DCM - CIRE), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Centrale Lille Institut (CLIL), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)
Rok vydání: 2013
Předmět:
Zdroj: Angewandte Chemie International Edition
Angewandte Chemie International Edition, 2014, 53 (6), pp.1654-1658. ⟨10.1002/anie.201308132⟩
Angewandte Chemie International Edition, Wiley-VCH Verlag, 2014, 53, pp.1654-1658. ⟨10.1002/anie.201308132⟩
ISSN: 1521-3773
1433-7851
DOI: 10.1002/anie.201308132⟩
Popis: The development of multicomponent molecular systems for the photocatalytic reduction of water to hydrogen has experienced considerable growth since the end of the 1970s. Recently, with the aim of improving the efficiency of the catalysis, single-component photocatalysts have been developed in which the photosensitizer is chemically coupled to the hydrogen-evolving catalyst in the same molecule through a bridging ligand. Until now, none of these photocatalysts has operated efficiently in pure aqueous solution: a highly desirable medium for energy-conversion applications. Herein, we introduce a new ruthenium-rhodium polypyridyl complex as the first efficient homogeneous photocatalyst for H2 production in water with turnover numbers of several hundred. This study also demonstrates unambiguously that the catalytic performance of such systems linked through a nonconjugated bridge is significantly improved as compared to that of a mixture of the separate components. Hydrogen evolution in water: An efficient homogeneous single-component Ru2Rh photocatalyst promoted H2 evolution in fully aqueous solution in the presence of ascorbate as a sacrificial electron donor with turnover numbers (TONs) up to 430 (see picture). The catalytic performance of the linked system with a nonconjugated bridge was significantly improved as compared to that of a mixture of the separate components.
Databáze: OpenAIRE