From Hydrogenases to Noble Metal–Free Catalytic Nanomaterials for H 2 Production and Uptake
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- 4 December 2009
- journal article
- research article
- Published by American Association for the Advancement of Science (AAAS) in Science
- Vol. 326 (5958), 1384-1387
- https://doi.org/10.1126/science.1179773
Abstract
Interconversion of water and hydrogen in unitized regenerative fuel cells is a promising energy storage framework for smoothing out the temporal fluctuations of solar and wind power. However, replacement of presently available platinum catalysts by lower-cost and more abundant materials is a requisite for this technology to become economically viable. Here, we show that the covalent attachment of a nickel bisdiphosphine–based mimic of the active site of hydrogenase enzymes onto multiwalled carbon nanotubes results in a high–surface area cathode material with high catalytic activity under the strongly acidic conditions required in proton exchange membrane technology. Hydrogen evolves from aqueous sulfuric acid solution with very low overvoltages (20 millivolts), and the catalyst exhibits exceptional stability (more than 100,000 turnovers). The same catalyst is also very efficient for hydrogen oxidation in this environment, exhibiting current densities similar to those observed for hydrogenase-based materials.Keywords
This publication has 26 references indexed in Scilit:
- Synthetic Support of De Novo Design: Sterically Bulky [FeFe]‐Hydrogenase ModelsAngewandte Chemie International Edition, 2008
- Carbon nanotubes—electronic/electrochemical properties and application for nanoelectronics and photonicsChemical Society Reviews, 2008
- Electrochemical grafting by reduction of 4-aminoethylbenzenediazonium salt: Application to the immobilization of (bio)moleculesElectrochemistry Communications, 2007
- Models for the Hydrogenases Put the Focus Where It Should Be—HydrogenAngewandte Chemie International Edition, 2007
- Investigating and Exploiting the Electrocatalytic Properties of HydrogenasesChemical Reviews, 2007
- Nature of hydrogen interactions with Ni(II) complexes containing cyclic phosphine ligands with pendant nitrogen basesProceedings of the National Academy of Sciences, 2007
- Attachment of organic layers to conductive or semiconductive surfaces by reduction of diazonium saltsChemical Society Reviews, 2005
- Transparent, Conductive Carbon Nanotube FilmsScience, 2004
- Crystal structure of the nickel–iron hydrogenase from Desulfovibrio gigasNature, 1995
- Carbon/poly {pyrrole-[(C5Me5)RhIII(bpy)Cl]+} modified electrodes; a molecularly-based material for hydrogen evolution (bpy = 2,2′-bipyridine)Journal of the Chemical Society, Chemical Communications, 1989