Microenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D2O

Meng He, Rui Li, Chuanqi Cheng, Cuibo Liu () and Bin Zhang ()
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Meng He: Tianjin University
Rui Li: Tianjin University
Chuanqi Cheng: Tianjin University
Cuibo Liu: Tianjin University
Bin Zhang: Tianjin University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract The high Faradaic efficiency (FE) of the electrocatalytic deuteration of organics with D2O 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 D2 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 D2O with an 80% FE at −100 mA cm−2. 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 D2 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−2 rationalizes the design concept.

Date: 2024
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DOI: 10.1038/s41467-024-49544-y

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