Journal
NATURE CHEMISTRY
Volume 13, Issue 6, Pages 523-+Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41557-021-00652-y
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Funding
- University of Zurich
- University Research Priority Program LightChEC
- Swiss National Science Foundation [PYAPP2 160586, CRSII2_160801]
- Swiss National Supercomputing Centre (CSCS) [uzh1, s965]
- INSPIRE potential master fellowship - SNSF NCCR-MARVEL
- LightChEC
- Swiss National Science Foundation (SNF) [CRSII2_160801, PYAPP2_160586] Funding Source: Swiss National Science Foundation (SNF)
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The study demonstrates a non-covalent 'click' chemistry approach to reversibly bind molecular electrocatalysts to electrode surfaces through host-guest complexation. This efficient method enables the replacement and reuse of molecular catalysts, enhancing the attractiveness of electrosynthetic systems.
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.
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