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用于从一氧化碳和一氧化氮电合成尿素的单原子铑合金化钴

Single-Atom Rh Alloyed Co for Urea Electrosynthesis from CO and NO.

作者信息

Wan Yuying, Zhang Zhuoyan, Qian Jinmei, Wei Yicheng, Kang Jilong, Chu Ke

机构信息

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

出版信息

Nano Lett. 2024 Sep 4;24(35):10928-10935. doi: 10.1021/acs.nanolett.4c02767. Epub 2024 Aug 20.

Abstract

Single-atom Rh alloyed Co (RhCo) is explored as an efficient catalyst for urea electrosynthesis via coelectrolysis of CO and NO (UECN). Theoretical calculations and in situ spectroscopic measurements unravel the synergetic effect of Co and Rh in promoting the UECN process, where the Rh site activates NO to form *NH, while the Co site activates CO to form *CO. The formed *CO then desorbs from the Co site and transfers to the Rh site, followed by continuous C-N coupling with *NH formed on the Rh site to synthesize urea. Remarkably, RhCo assembled in a flow cell delivers the exceptional urea yield rate of 24.9 mmol h g and Faradaic efficiency of 51.1%, outperforming most previously reported UECN catalysts.

摘要

单原子铑合金化钴(RhCo)被探索作为一种通过CO和NO共电解合成尿素(UECN)的高效催化剂。理论计算和原位光谱测量揭示了Co和Rh在促进UECN过程中的协同作用,其中Rh位点激活NO形成NH,而Co位点激活CO形成CO。形成的CO然后从Co位点解吸并转移到Rh位点,随后与在Rh位点形成的NH进行连续的C-N偶联以合成尿素。值得注意的是,组装在流动池中的RhCo实现了24.9 mmol h g的优异尿素产率和51.1%的法拉第效率,优于大多数先前报道的UECN催化剂。

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