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Issue 13, 2018
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Comprehensive reaction mechanisms at and near the Ni–Fe active sites of [NiFe] hydrogenases

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Abstract

[NiFe] hydrogenase (H2ase) catalyzes the oxidation of dihydrogen to two protons and two electrons and/or its reverse reaction. For this simple reaction, the enzyme has developed a sophisticated but intricate mechanism with heterolytic cleavage of dihydrogen (or a combination of a hydride and a proton), where its Ni–Fe active site exhibits various redox states. Recently, thermodynamic parameters of the acid–base equilibrium for activation–inactivation, a new intermediate in the catalytic reaction, and new crystal structures of [NiFe] H2ases have been reported, providing significant insights into the activation–inactivation and catalytic reaction mechanisms of [NiFe] H2ases. This Perspective provides an overview of the reaction mechanisms of [NiFe] H2ases based on these new findings.

Graphical abstract: Comprehensive reaction mechanisms at and near the Ni–Fe active sites of [NiFe] hydrogenases

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Article information


Submitted
28 Dec 2017
Accepted
20 Feb 2018
First published
21 Feb 2018

Dalton Trans., 2018,47, 4408-4423
Article type
Perspective

Comprehensive reaction mechanisms at and near the Ni–Fe active sites of [NiFe] hydrogenases

H. Tai, Y. Higuchi and S. Hirota, Dalton Trans., 2018, 47, 4408
DOI: 10.1039/C7DT04910B

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