Issue 8, 2024

A cross-metathesis approach for polymetallic [FeFe]-hydrogenase mimics

Abstract

A method has been developed for synthesizing [FeFe]-H2ase mimics with diverse structures and properties, employing cross-metathesis of olefins. Vinylmetallocenes (5 and 6) and vinyl half-sandwich complexes (10 and 11) have been used as cross-metathesis partners with [FeFe]-H2ase mimics (4, 8, and 9) bearing a double bond in the moiety attached to the ADT-bridge nitrogen. Electrochemical studies of these complexes, encompassing metallocene-type (7a–b, 12a–b, and 13a–b) as well as half-sandwich derivatives (12c and 13c–d), have demonstrated that the introduction of a redox unit has a marginal impact on the reduction potential of these [FeFe]-H2ase mimics. The application of this cross-metathesis approach has allowed the synthesis of [FeFe]-H2ase mimics featuring an Ir(III) electrochemical antenna (16–18) as well as systems having an electron-donor-photosensitizer structure (ED-PS) (23). The electrocatalytic properties of these complexes have been elucidated through electrochemical studies.

Graphical abstract: A cross-metathesis approach for polymetallic [FeFe]-hydrogenase mimics

Supplementary files

Article information

Article type
Paper
Submitted
26 dec 2023
Accepted
22 jan 2024
First published
24 jan 2024
This article is Open Access
Creative Commons BY license

Dalton Trans., 2024,53, 3756-3764

A cross-metathesis approach for polymetallic [FeFe]-hydrogenase mimics

S. Aguado, P. García-Álvarez, J. A. Cabeza, L. Casarrubios and M. A. Sierra, Dalton Trans., 2024, 53, 3756 DOI: 10.1039/D3DT04197B

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