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Hydrogen Evolution from Aqueous Solutions Mediated by a Heterogenized [NiFe]-Hydrogenase Model: Low pH Enables

Md Estak Ahmed¹, Samir Chattopadhyay¹, Lianke Wang²

¹Indian Association for the Cultivation of Science, 700032, Kolkata, India.

Angewandte Chemie (International Ed. in English)

|October 12, 2018

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.

Keywords:

[NiFe]-hydrogenase electrocatalysis heterogeneous catalysis hydrogen evolution reaction mechanism

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