Electrocatalysis is an appealing approach complementary to thermocatalysis for redox organic transformations due to the potential low-energy cost and facile control in reaction rate and selectivity through the manipulation of electrocatalytic parameters. Molecular electrocatalysts allows in-depth mechanistic studies in a relatively convenient manner because of the well-defined active sites at a molecular level, however they typically suffer from complex synthesis and low utilization efficiency during electrocatalysis. On the other hand, solid-state electrocatalysts usually exhibit better efficiency and durability, but it is challenging in elucidating their working mechanisms due to the lack of the molecular structure information of the active sites. Herein, we present a hybrid strategy to introduce polymeric multi-dentate ligands coated on conductive substrates via photo-induced polymerization. The resulting ligand film enables us to obtain transition metal-containing electrocatalysts with unsaturated coordination spheres, which cannot be achieved readily in homogeneous catalysis. These hybrid electrocatalysts exhibit excellent activity and durability for a wide array of redox organic reactions, including alcohol oxidation and Achmatowicz rearrangement.

Immobilized polymeric electrocatalysts for redox organic reactions

2019 Spring National Meeting

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