Overcoming Electrostatic Interaction via Pulsed Electroreduction for Boosting the Electrocatalytic Urea Synthesis

Angew Chem Int Ed Engl. 2024 Apr 10:e202402684. doi: 10.1002/anie.202402684. Online ahead of print.ABSTRACTElectrocatalytic urea synthesis under ambient conditions offers a promising alternative strategy to the traditional energy-intensive urea industry protocol. Limited by the electrostatic interaction, the reduction reaction of anions at the cathode in the electrocatalytic system is not easily achievable. Here, we propose a novel strategy to overcome electrostatic interaction via pulsed electroreduction. We found that the reconstruction-resistant CuSiOx nanotube, with abundant atomic Cu-O-Si interfacial sites, exhibits ultrastability in the electrosynthesis of urea from nitrate and CO2. Under a pulsed potential approach with optimal operating conditions, the Cu-O-Si interfaces achieve a superior urea production rate (1606.1 μg h-1 mgcat.-1) with high selectivity (79.01%) and stability (the Faradaic efficiency is retained at 80% even after 80 h of testing), outperforming most reported electrocatalytic synthesis urea catalysts. We believe our strategy will incite further investigation into pulsed electroreduction increasing substrate transport, which may guide the design of ambient urea electrosynthesis and other energy conversion systems.PMID:38597346 | DOI:10.1002/anie.202402684
Source: Angewandte Chemie - Category: Chemistry Authors: Source Type: research