Immobilization of molecular catalysts on electrode surfaces using host–guest interactions

Abstract

Anchoring molecular catalysts on electrode surfaces combines the high selectivity and activity of molecular systems with the practicality of heterogeneous systems. Molecular catalysts, however, are far less stable than traditional heterogeneous electrocatalysts, and therefore a method to easily replace anchored molecular catalysts that have degraded could make such electrosynthetic systems more attractive. Here we applied a non-covalent ‘click’ chemistry approach to reversibly bind molecular electrocatalysts to electrode surfaces through host–guest complexation with surface-anchored cyclodextrins. The host–guest interaction is remarkably strong and enables the flow of electrons between the electrode and the guest catalyst. Electrosynthesis in both organic and aqueous media was demonstrated on metal oxide electrodes, with stability on the order of hours. The catalytic surfaces can be recycled by controlled release of the guest from the host cavities and the readsorption of fresh guest. Molecular catalysts can be made more practical by anchoring them onto electrode surfaces, but such systems are less stable than standard heterogeneous electrocatalysts. Now, supramolecular hosts bound to electrode surfaces have enabled the immobilization of molecular electrocatalysts through host–guest interactions. Desorbed or degraded guest molecules can be replaced with fresh guest molecules, extending their lifetimes.

Cite this article

Sévery, L., Szczerbiński, J., Taskin, M. et al. Immobilization of molecular catalysts on electrode surfaces using host–guest interactions. Nat. Chem. (2021). https://doi.org/10.1038/s41557-021-00652-y

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