Hydrogen Evolution from Aqueous Solutions Mediated by a Heterogenized [NiFe]‐Hydrogenase Model: Low pH Enables Catalysis through an Enzyme‐Relevant Mechanism. Issue 49 (11th November 2018)

• Record Type: Journal Article
• Authors: Ahmed, Md Estak; Chattopadhyay, Samir; Wang, Lianke; Brazzolotto, Deborah; Pramanik, Debajyoti; Aldakov, Dmitry; Fize, Jennifer; Morozan, Adina; Gennari, Marcello; Duboc, Carole; Dey, Abhishek; Artero, Vincent
• Is Part Of: Angewandte Chemie international edition. Volume 57:Issue 49(2018)
• Page Start: 16001
• Page End: 16004
• Publication Date: 2018-11-11
• Subjects: electrocatalysis -- heterogeneous catalysis -- hydrogen evolution -- [NiFe]-hydrogenase -- reaction mechanism; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201808215
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: [NiFe]‐hydrogenase enzymes are efficient catalysts for H2 evolution but their synthetic models have not been reported to be active under aqueous conditions so far. Here we show that a close model of the [NiFe]‐hydrogenase active site can work as a very active and stable heterogeneous H2 evolution catalyst under mildly acidic aqueous conditions. Entry in catalysis is a Ni I Fe II complex, with electronic structure analogous to the Ni‐L state of the enzyme, corroborating the mechanism modification recently proposed for [NiFe]‐hydrogenases. Abstract : Learning from nature : [NiFe]‐hydrogenase enzymes are efficient catalysts for H2 evolution but their synthetic models have not been reported to be active under aqueous conditions so far. A close model of the [NiFe]‐hydrogenase active site (see picture) is now shown to operate as a very active and stable heterogeneous H2 evolution catalyst under mildly acidic aqueous conditions.