Surfactant-enhanced Cuδ+ and induced electrostatic forces promote the electrocatalytic deuteron-dechlorination of trichloroacetic acid
Year: 2025
Type: article
Abstract: Electrocatalytic deuteron-dechlorination of trichloroacetic acid (TCAA) in D2O provides a green route to synthesize commercial acetic-d3 acid-d (AA-d4). Synthesizing AA-d4 with a high Faradaic efficiency (FE) and reaction rate is highly challenging because of the difficult C-Cl bond deuteration of the 2-monochloroacetic-2,2-d2 acid-d (MCAA-d3) intermediate. Here, a quaternary ammonium salt surfactant-modified low-coordination copper electrocatalyst was designed, achieving TCAA-to-AA-d4 with a 91% selectivity, 91% FE and 0.59 mmol h−1 reaction rate at -100 mA cm−2. Mechanistic and kinetics studies reveal that the surfactant enhances the adsorption of MCAA-d3 through the electrostatic force and heightens the electron deficiency of Cuδ+ sites, which accelerates the electron transfer and promotes the C-Cl bond activation, increasing the AA-d4 selectivity. Surfactant-caused low D2O coverage suppresses D2 formation, improving the FE. 1.84 g AA-d4 electrosynthesis with a 30 mmol h−1 reaction rate and 65% FE at 600 mA cm−2 and deuterated drug applications demonstrate promising potential.
Source: Nature Communications
Institution: Tianjin University
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $6,990
Awards: G256199584, G8462641205
OpenAlex ID: W4416576100
