NDLI: $[Rh^{III}(dmbpy)_{2}Cl_{2}]^{+}$ as a Highly Efficient Catalyst for Visible-Light-Driven Hydrogen Production in Pure Water: Comparison with Other Rhodium $Catalysts^{†}$

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$[Rh^{III}(dmbpy)_{2}Cl_{2}]^{+}$ as a Highly Efficient Catalyst for Visible-Light-Driven Hydrogen Production in Pure Water: Comparison with Other Rhodium $Catalysts^{†}$

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$[Rh^{III}(dmbpy)_{2}Cl_{2}]^{+}$ as a Highly Efficient Catalyst for Visible-Light-Driven Hydrogen Production in Pure Water: Comparison with Other Rhodium $Catalysts^{†}$

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Fortage, Jérôme Odobel, Fabrice Rebarz, Mateusz Collomb, Marie-noëlle Sliwa, Michel Chauvin, Jérôme Poizat, Olivier Deronzier, Alain Gennari, Marcello Stoll, Thibaut Serrano, Isabel
Description	Author Affiliation: Stoll T ( Université Joseph Fourier Grenoble 1/CNRS, Département de Chimie Moléculaire, UMR 5250, Institut de Chimie Moléculaire de Grenoble, FR-CNRS-2607, Laboratoire de Chimie Inorganique Rédox, BP 53, 38041 Grenoble Cedex 9, France.)
Abstract	We report a very efficient homogeneous system for the visible-light-driven hydrogen production in pure aqueous solution at room temperature. This comprises $[Rh^{III}(dmbpy)_{2}Cl_{2}]Cl$ (1) as catalyst, $[Ru(bpy)_{3}]Cl_{2}$ (PS1) as photosensitizer, and ascorbate as sacrificial electron donor. Comparative studies in aqueous solutions also performed with other known rhodium catalysts, or with an iridium photosensitizer, show that 1) the PS1/1/ascorbate/ascorbic acid system is by far the most active rhodium-based homogeneous photocatalytic system for hydrogen production in a purely aqueous medium when compared to the previously reported rhodium catalysts, $Na_{3}[Rh^{I}(dpm)_{3}Cl]$ and $[Rh^{III}(bpy)Cp*(H_{2}O)]SO_{4}$ and 2) the system is less efficient when $[Ir^{III}(ppy)_{2}(bpy)]Cl$ (PS2) is used as photosensitizer. Because catalyst 1 is the most efficient rhodium-based $H_{2}-evolving$ catalyst in water, the performance limits of this complex were further investigated by varying the PS1/1 ratio at pH 4.0. Under optimal conditions, the system gives up to 1010 turnovers versus the catalyst with an initial turnover frequency as high as $857 TON h^{−1}.$ Nanosecond transient absorption spectroscopy measurements show that the initial step of the photocatalytic $H_{2}-evolution$ mechanism is a reductive quenching of the PS1 excited state by ascorbate, leading to the reduced form of PS1, which is then able to reduce $[Rh^{III}(dmbpy)_{2}Cl_{2}]^{+}$ to $[Rh^{I}(dmbpy)_{2}]^{+}.$ This reduced species can react with protons to yield the hydride $[Rh^{III}(H)(dmbpy)_{2}(H_{2}O)]^{2+},$ which is the key intermediate for the $H_{2}$ production.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	2
Volume Number	19
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2013-01-07
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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