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

Area of Science:

• Electrochemistry
• Organic Synthesis
• Materials Science

Background:

• Electrocatalytic deuteration is crucial for producing deuterated compounds.
• A major challenge is the trade-off between Faradaic efficiency (FE) and current density due to competing deuterium (D2) evolution.
• Achieving high FE at industrial current densities remains difficult.

Purpose of the Study:

• To develop a strategy for high Faradaic efficiency (FE) electrocatalytic deuteration at large current densities.
• To overcome the inherent trade-off between FE and current density in deuteration reactions.
• To demonstrate a novel approach for enhanced deuteration of arylacetonitrile.

Main Methods:

• Utilizing a nanotip-enhanced electric field to concentrate reactants.
• Employing a surfactant-modified interface to create a deuterophobic microenvironment.
• Investigating the electrocatalytic deuteration of arylacetonitrile in heavy water (D2O).

Main Results:

• Achieved an 80% Faradaic efficiency (FE) for arylacetonitrile deuteration at a high current density of -100 mA cm⁻².
• The nanotip electric field increased arylacetonitrile concentration and lowered activation energy.
• The surfactant-modified interface accelerated reactant transfer and suppressed deuterium evolution.

Conclusions:

• The combined nanotip electric field and surfactant interface effectively breaks the FE-current density trade-off.
• This strategy enables efficient electrocatalytic deuteration at industrially relevant current densities.
• The approach shows promise for broader applications in deuteration reactions.