Reversible Electrocatalytic Production and Oxidation of Hydrogen at Low Overpotentials by a Functional Hydrogenase Mimic

An efficient ligand combination: A new bis(diphosphine) nickel(II) complex (see picture) is described. A ΔG° value of 0.84 kcal mol−1 for hydrogen addition for this complex was calculated from the experimentally determined equilibrium constant. This complex displayed reversible electrocatalytic acti...

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Veröffentlicht in:	Angewandte Chemie (International ed.) 2012-03, Vol.51 (13), p.3152-3155
Hauptverfasser:	Smith, Stuart E., Yang, Jenny Y., DuBois, Daniel L., Bullock, R. Morris
Format:	Artikel
Sprache:	eng
Schlagworte:	08 HYDROGEN ACETONITRILE ACTIVE-SITES Biomimetic Materials - chemistry CATALYSIS CATALYSTS Chemical equilibrium COMPLEXES Coordination Complexes - chemistry ELECTROCHEMISTRY ENZYMES FUNCTIONALS H-2 PRODUCTION HOMOGENEOUS CATALYSIS HYDROGEN Hydrogen - chemistry HYDROGEN ADDITIONS HYDROGEN PRODUCTION Hydrogenase Hydrogenase - chemistry hydrogenase enzymes HYDROGENASES IRON-ONLY HYDROGENASE Ligands MATERIALS SCIENCE Mathematical analysis MOLECULAR ELECTROCATALYSTS Nickel - chemistry OXIDATION Oxidation-Reduction PENDANT BASES Phosphines - chemistry Pictures PRODUCTION REACTIVITY Thermodynamics
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Zusammenfassung:	An efficient ligand combination: A new bis(diphosphine) nickel(II) complex (see picture) is described. A ΔG° value of 0.84 kcal mol−1 for hydrogen addition for this complex was calculated from the experimentally determined equilibrium constant. This complex displayed reversible electrocatalytic activity for hydrogen production and oxidation at low overpotentials, which are characteristic for hydrogenase enzymes.
ISSN:	1433-7851 1521-3773
DOI:	10.1002/anie.201108461