赣南师范大学张勇团队报道了通过脉冲电还原克服静电相互作用促进电催化尿素合成。相关研究成果发表在2024年4月10日出版的《德国应用化学》。

环境条件下的电催化尿素合成为传统的能源密集型尿素工业方案，提供了一种很有前途的替代策略。受静电相互作用的限制，在电催化系统中，阴离子在阴极的还原反应不容易实现。

该文中，研究人员提出了一种通过脉冲电还原克服静电相互作用的新策略。研究发现，具有丰富的Cu-O-Si原子界面位点的耐重构CuSiOx纳米管，在由硝酸盐和CO₂电合成尿素中表现出超稳定性。在具有最佳操作条件的脉冲电位方法下，Cu-O-Si界面实现了优异的尿素产率（1606.1μg h^-1 mgcat.^-1），具有高选择性（79.01%）和稳定性（即使在测试80小时后，法拉第效率仍保持在80%），优于大多数报道的电催化合成尿素催化剂。

该策略将促进对脉冲电还原增加底物传输的进一步研究，这可能指导环境尿素电合成和其他能量转换系统的设计。

附：英文原文

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

Author: Weibin Qiu, Shimei Qin, Yibao Li, Ning Cao, Weirong Cui, Zedong Zhang, Zechao Zhuang, Dingsheng Wang, Yong Zhang

Issue&Volume: 2024-04-10

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 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.

DOI: 10.1002/anie.202402684

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202402684