Zhang Ying, Li Zhuohang, Qiang Chaofan, Chen Kai, Guo Yali, Chu Ke
School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou 730070, China.
ACS Nano. 2024 Sep 10;18(36):25316-25324. doi: 10.1021/acsnano.4c09141. Epub 2024 Aug 26.
Urea electrosynthesis from coelectrolysis of NO and CO (UENC) holds a significant prospect to achieve efficient and sustainable urea production. Herein, atomically dispersed Cu on InO (Cu/InO) is designed as an effective and robust catalyst for the UENC. Combined theoretical calculations and in situ spectroscopic analysis reveal the synergistic effect of the Cu-O-In site and the In site to boost the UENC energetics via a relay catalysis pathway, where the Cu-O-In site drives *NO → *NH and the In site catalyzes *CO → *CO. The generated *CO is then migrated from the In site to the Cu-O-In site, followed by C-N coupling with *NH on the Cu-O-In site to generate urea. Consequently, Cu/InO assembled within a flow cell exhibits an impressive urea yield rate of 28.97 mmol h g with a urea-Faradaic efficiency (FE) of 50.88%.
通过一氧化氮和一氧化碳共电解进行尿素电合成(UENC)在实现高效且可持续的尿素生产方面具有重大前景。在此,氧化铟负载的原子分散铜(Cu/InO)被设计为一种用于UENC的高效且稳定的催化剂。结合理论计算和原位光谱分析揭示了Cu-O-In位点和In位点的协同效应,通过接力催化途径促进UENC的能量学过程,其中Cu-O-In位点驱动NO→NH,In位点催化CO→CO。生成的CO随后从In位点迁移至Cu-O-In位点,接着在Cu-O-In位点上与NH进行C-N偶联以生成尿素。因此,在流动池中组装的Cu/InO表现出令人印象深刻的尿素产率,为28.97 mmol h g,尿素法拉第效率(FE)为50.88%。