Heterogenization of a Water-Insoluble Molecular Complex for Catalysis of the Proton-Reduction Reaction in Highly Acidic Aqueous Solutions

Abstract

Our long-held interest in the resiliency of electrochemical functionalities upon surface immobilization has herded us from directly chemisorbed electroactive moieties, to anchor group-leashed redox-active couples and to surface-tethered enzyme-inspired molecular catalysts. The latter represent the most intricate because the electrocatalytic activities involve mixed-valence states and may require certain entatic (fractionally rotated) configurations. In this regard, we recently investigated the proton-reduction electrocatalysis by hydrogenase-inspired di-iron complexes at polycrystalline and (111)-faceted Au electrodes.