Immobilization of molecular catalysts on electrode surfaces using host-guest interactions.

Autor: Sévery L; Department of Chemistry, University of Zurich, Zurich, Switzerland.; Department of Chemistry, University of California, Berkeley, CA, USA., Szczerbiński J; Laboratory of Organic Chemistry, ETH Zurich, Zurich, Switzerland., Taskin M; Department of Physics, University of Zurich, Zurich, Switzerland., Tuncay I; Department of Chemistry, University of Zurich, Zurich, Switzerland., Brandalise Nunes F; Department of Chemistry, University of Zurich, Zurich, Switzerland., Cignarella C; Department of Chemistry, University of Zurich, Zurich, Switzerland., Tocci G; Department of Chemistry, University of Zurich, Zurich, Switzerland., Blacque O; Department of Chemistry, University of Zurich, Zurich, Switzerland., Osterwalder J; Department of Physics, University of Zurich, Zurich, Switzerland., Zenobi R; Laboratory of Organic Chemistry, ETH Zurich, Zurich, Switzerland., Iannuzzi M; Department of Chemistry, University of Zurich, Zurich, Switzerland., Tilley SD; Department of Chemistry, University of Zurich, Zurich, Switzerland. david.tilley@chem.uzh.ch.
Jazyk: angličtina
Zdroj: Nature chemistry [Nat Chem] 2021 Jun; Vol. 13 (6), pp. 523-529. Date of Electronic Publication: 2021 Mar 25.
DOI: 10.1038/s41557-021-00652-y
Abstrakt: 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.
Databáze: MEDLINE
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