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<p>Electrocatalytic deuteron-dechlorination of trichloroacetic acid (TCAA) in D<sub>2</sub>O provides a green route to synthesize commercial acetic-<i>d</i><sub>3</sub> acid-<i>d</i> (AA-<i>d</i><sub>4</sub>). Synthesizing AA-<i>d</i><sub>4</sub> 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-<i>d</i><sub>2</sub> acid-<i>d</i> (MCAA-<i>d</i><sub>3</sub>) intermediate. Here, a quaternary ammonium salt surfactant-modified low-coordination copper electrocatalyst is designed, achieving TCAA-to-AA-<i>d</i><sub>4</sub> with a 91% selectivity, 91% FE and 0.59 mmol h<sup>−1</sup> reaction rate at −100 mA cm<sup>−2</sup>. Mechanistic and kinetic studies reveal that the surfactant enhances the adsorption of MCAA-<i>d</i><sub>3</sub> through electrostatic forces and increases the electron deficiency of Cu<sup>δ+</sup> sites, which accelerates electron transfer and promotes C−Cl bond activation, increasing the AA-<i>d</i><sub>4</sub> selectivity. Surfactant-induced low D<sub>2</sub>O coverage suppresses D<sub>2</sub> formation, improving the FE. AA-<i>d</i><sub>4</sub> electrosynthesis (1.84 g) with a 30 mmol h<sup>−1</sup> reaction rate and 65% FE at 600 mA cm<sup>−2</sup> and deuterated drug applications demonstrate promising potential.</p>

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Surfactant-enhanced Cuδ+ and induced electrostatic forces promote the electrocatalytic deuteron-dechlorination of trichloroacetic acid

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月24日

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  • Mengmei Qin,
  • Meng He,
  • Chuanqi Cheng,
  • Rui Li,
  • Cuibo Liu,
  • Bin Zhang

摘要

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 is 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 kinetic studies reveal that the surfactant enhances the adsorption of MCAA-d3 through electrostatic forces and increases the electron deficiency of Cuδ+ sites, which accelerates electron transfer and promotes C−Cl bond activation, increasing the AA-d4 selectivity. Surfactant-induced low D2O coverage suppresses D2 formation, improving the FE. AA-d4 electrosynthesis (1.84 g) with a 30 mmol h−1 reaction rate and 65% FE at 600 mA cm−2 and deuterated drug applications demonstrate promising potential.