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负载于氧化铟上的原子级分散铜用于硝酸盐和一氧化碳中继电催化转化为尿素

Atomically Dispersed Cu on InO for Relay Electrocatalytic Conversion of Nitrate and CO to Urea.

作者信息

Zhang Ying, Li Zhuohang, Qiang Chaofan, Chen Kai, Guo Yali, Chu Ke

机构信息

School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou 730070, China.

出版信息

ACS Nano. 2024 Sep 10;18(36):25316-25324. doi: 10.1021/acsnano.4c09141. Epub 2024 Aug 26.

Abstract

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%.

摘要

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%。

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