Premium
Direct Comparison of the Performance of a Bio‐inspired Synthetic Nickel Catalyst and a [NiFe]‐Hydrogenase, Both Covalently Attached to Electrodes
Author(s) -
RodriguezMaciá Patricia,
Dutta Arnab,
Lubitz Wolfgang,
Shaw Wendy J.,
Rüdiger Olaf
Publication year - 2015
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201502364
Subject(s) - hydrogenase , overpotential , catalysis , nickel , enzyme , combinatorial chemistry , covalent bond , electrode , chemistry , materials science , chemical engineering , nanotechnology , biochemistry , electrochemistry , organic chemistry , engineering
The active site of hydrogenases has been a source of inspiration for the development of molecular catalysts. However, direct comparisons between molecular catalysts and enzymes have not been possible because different techniques are used to evaluate both types of catalysts, minimizing our ability to determine how far we have come in mimicking the enzymatic performance. The catalytic properties of the [Ni(P Cy 2 N Gly 2 ) 2 ] 2+ complex with the [NiFe]‐hydrogenase from Desulfovibrio vulgaris immobilized on a functionalized electrode were compared under identical conditions. At pH 7, the enzyme shows higher activity and lower overpotential with better stability, while at low pH, the molecular catalyst outperforms the enzyme in all respects. This is the first direct comparison of enzymes and molecular complexes, enabling a unique understanding of the benefits and detriments of both systems, and advancing our understanding of the utilization of these bio‐inspired complexes in fuel cells.