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

Weibin Qiu, Shimei Qin, Yibao Li, Ning Cao, Wei‐Rong Cui, Zedong Zhang, Zechao Zhuang, Dingsheng Wang, Yong Zhang, Yong Zhang

2024Angewandte Chemie International Edition170 citationsDOI

Abstract

Abstract Electrocatalytic 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 CuSiO x nanotube, with abundant atomic Cu−O−Si interfacial sites, exhibits ultrastability in the electrosynthesis of urea from nitrate and CO 2 . 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 mg cat. −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.

Topics & Concepts

Boosting (machine learning)UreaElectrochemistryElectrocatalystElectrostatic interactionMaterials scienceChemistryInorganic chemistryChemical engineeringElectrodeComputer scienceChemical physicsPhysical chemistryOrganic chemistryArtificial intelligenceEngineeringAmmonia Synthesis and Nitrogen ReductionCaching and Content DeliveryCO2 Reduction Techniques and Catalysts