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Light-Driven Hydrogen Production from Aqueous Protons using Molybdenum Catalysts
Abstract
Homogeneous light-driven systems employing molecular molybdenum catalysts for hydrogen production are described. The specific Mo complexes studied are six-coordinate bis(benzenedithiolate) derivatives having two additional isocyanide or phosphine ligands to complete the coordination sphere. Each of the complexes possesses a trigonal prismatic coordination geometry. The complexes were investigated as proton reduction catalysts in the presence of [Ru(bpy)<sub>3</sub>]<sup>2+</sup>, ascorbic acid, and visible light. Over 500 TON are obtained over 24 h. Electrocatalysis occurs between the Mo<sup>IV</sup>/Mo<sup>III</sup> and Mo<sup>III</sup>/Mo<sup>II</sup> redox couples, around 1.0 V vs SCE. Mechanistic studies by <sup>1</sup>H NMR spectroscopy show that upon two-electron reduction the Mo(CNR)<sub>2</sub>(bdt)<sub>2</sub> complex dissociates the isocyanide ligands, followed by addition of acid to result in the formation of molecular hydrogen and the Mo(bdt)<sub>2</sub> complex- Text
- Journal contribution
- Biochemistry
- Cell Biology
- Biotechnology
- Marine Biology
- Cancer
- Computational Biology
- Biological Sciences not elsewhere classified
- Chemical Sciences not elsewhere classified
- Physical Sciences not elsewhere classified
- Aqueous Protons
- Mo complexes
- 1.0 V vs SCE
- molybdenum catalysts
- Mechanistic studies
- hydrogen production
- 24 h
- prismatic coordination geometry
- 1 H NMR spectroscopy show
- isocyanide ligands
- proton reduction catalysts
- phosphine ligands
- coordination sphere
- acid
- 500 TON
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Last time updated on 12/02/2018
This paper was published in The Francis Crick Institute.
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