Microenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D<sub>2</sub>O.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38898044.
- Also identified by DOI 10.1038/s41467-024-49544-y and PMC identifier 11187139.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
The high Faradaic efficiency (FE) of the electrocatalytic deuteration of organics with D<sub>2</sub>O at a large current density is significant for deuterated electrosynthesis. However, the FE and current density are the two ends of a seesaw because of the severe D<sub>2</sub> evolution side reaction at nearly industrial current densities. Herein, we report a combined scenario of a nanotip-enhanced electric field and surfactant-modified interface microenvironment to enable the electrocatalytic deuteration of arylacetonitrile in D<sub>2</sub>O with an 80% FE at -100 mA cm<sup>-2</sup>. The increased concentration with low activation energy of arylacetonitrile due to the large electric field along the tips and the accelerated arylacetonitrile transfer and suppressed D<sub>2</sub> evolution by the surfactant-created deuterophobic microenvironment contribute to breaking the trade-off between a high FE and large current density. Furthermore, the application of our strategy in other deuteration reactions with improved Faradaic efficiencies at -100 mA cm<sup>-2</sup> rationalizes the design concept.