Di-Iron Analogue of [FeFe]-Hydrogenase Active Site as a Molecular Electro-catalyst for Proton Reduction
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Di‑Iron Analogue of [FeFe]‑Hydrogenase Active Site as a Molecular Electro‑catalyst for Proton Reduction Xia Zhang1,2 · Lihong Liu1,2 · Weiming Cao1 · Dongjun Lv3 Received: 29 January 2020 / Accepted: 1 May 2020 © Springer Science+Business Media, LLC, part of Springer Nature 2020
Abstract With Me3NO being present, the ligand substitution reaction of [ (μ-dmedt){Fe (CO)3}2] by 4,4′-bipyridine afforded a new diiron complex (μ-dmedt)Fe2 (CO)5 (4,4′-bipyridine) 1, which was detected using IR, 1H NMR, elemental and MS analyses. Our electrochemical tests showed that compound 1 is capable to catalyze hydrogen production, which served as an efficient molecular electro-catalyst in the CH3CN solution or adsorbed on the surface of electrode for electrochemical generation of molecular hydrogen from HOAc or aqueous media. The relevance of these studies for designing efficient hydrogenase models lies in providing insights into the core of stereo-electronic features. Graphic Abstract A novel complex (μ-dmedt)Fe2 (CO)5 (4,4′-bipyridine) 1 bearing a functional groups have been prepared, which served as an efficient molecular electro-catalyst in the C H3CN solution or chemisorbed on the surface of electrode for electrochemical generation of molecular hydrogen from HOAC or aqueous media. Those will be of relevance to the natural system and crucial to the potential industrial application.
Keywords [FeFe]-hydrogenase active site · Molecular electro-catalyst · Hydrogen generation
1 Introduction Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10562-020-03248-2) contains supplementary material, which is available to authorized users. * Xia Zhang [email protected] * Lihong Liu [email protected] Extended author information available on the last page of the article
With the global energy demand and increasingly severe environmental problems, the use of clean, efficient and reproducible energy substitute for fossil fuels is being actively promoted as the ideal solution to overcome the shortage of energy as well as to tackle the greenhouse effect. Hydrogen (H2) is an ideal energy because it is clean, efficient and renewable. The photochemical or electrochemical generation
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of H2 is regarded as an efficient method to address the situation [1, 2]. Natural occurrence of hydrogenase enzymes is widespread among the microorganisms. Efficiently catalyzing the H + reduction to produce H2 by hydrogenase enzymes which can be classified as [Fe]-hydrogenase, [NiFe]-hydrogenase and [FeFe]-hydrogenase. The latter one, [FeFe]-hydrogenase, exhibits the strongest catalytic capability towards H+ reduction of proton to hydrogen [3]. The drawback though, is the difficulty in obtaining hydrogenase enzymes in sufficient amounts suitable for commercial usage and their instability outside the native environment [4–6]. In order to resolve this issue many research groups, ours being one of them, have introduced some good donor ligands into the model complexes by the way of CO-
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