Single-Atom Rh<sub>1</sub> Alloyed Co for Urea Electrosynthesis from CO<sub>2</sub> and NO<sub>3</sub><sup></sup>.

Wan, Yuying; Zhang, Zhuoyan; Qian, Jinmei; Wei, Yicheng; Kang, Jilong; Chu, Ke · Nano Lett · 2024

basic_science · Level V

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Abstract

Single-atom Rh<sub>1</sub> alloyed Co (Rh<sub>1</sub>Co) is explored as an efficient catalyst for urea electrosynthesis via coelectrolysis of CO<sub>2</sub> and NO<sub>3</sub><sup>-</sup> (UECN). Theoretical calculations and in situ spectroscopic measurements unravel the synergetic effect of Co and Rh<sub>1</sub> in promoting the UECN process, where the Rh<sub>1</sub> site activates NO<sub>3</sub><sup>-</sup> to form *NH<sub>2</sub>, while the Co site activates CO<sub>2</sub> to form *CO. The formed *CO then desorbs from the Co site and transfers to the Rh<sub>1</sub> site, followed by continuous C-N coupling with *NH<sub>2</sub> formed on the Rh<sub>1</sub> site to synthesize urea. Remarkably, Rh<sub>1</sub>Co assembled in a flow cell delivers the exceptional urea yield rate of 24.9 mmol h<sup>-1</sup> g<sup>-1</sup> and Faradaic efficiency of 51.1%, outperforming most previously reported UECN catalysts.