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Hydrogen Evolution from Aqueous Solutions Mediated by a Heterogenized [NiFe]‐Hydrogenase Model: Low pH Enables Catalysis through an Enzyme‐Relevant Mechanism
Author(s) -
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
Publication year - 2018
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.201808215
Subject(s) - hydrogenase , aqueous solution , catalysis , active site , chemistry , enzyme , combinatorial chemistry , enzyme catalysis , inorganic chemistry , photochemistry , organic chemistry
[NiFe]‐hydrogenase enzymes are efficient catalysts for H 2 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 H 2 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.