Boosting Electrochemical Urea Synthesis via Constructing Ordered Pd–Zn Active Pair  

作　　者：Weiliang Zhou Chao Feng Xuan Li Xingxing Jiang Lingyan Jing Shuai Qi Qihua Huo Miaoyuan Lv Xinbao Chen Tianchi Huang Jingwen Zhao Na Meng Hengpan Yang Qi Hu Chuanxin He 

机构地区：[1]College of Chemistry and Environmental Engineering,Shenzhen University,Shenzhen 518060,Guangdong,People’s Republic of China [2]School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering,Shihezi University,Shihezi 832003,Xinjiang,People’s Republic of China

出　　处：《Nano-Micro Letters》2024年第11期529-540,共12页纳微快报（英文版）

基　　金：supported by the National Natural Science Foundation of China(22379100,U21A20312);the Shenzhen Science and Technology Program(Grant No.20231121200418001);the Guangdong Basic and Applied Basic Research Foundation(2022B1515120084);the Key Project of Department of Education of Guangdong Province(2023ZDZX3020)。

摘　　要：Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained limited.Here,we report an atomically ordered intermetallic pallium-zinc(PdZn)electrocatalyst comprising a high density of PdZn pairs for boosting urea electrosynthesis.It is found that Pd and Zn are responsible for the adsorption and activation of NO_(3)^(-)and CO_(2),respectively,and thus the co-adsorption and co-activation NO_(3)^(-)and CO_(2) are achieved in ordered PdZn pairs.More importantly,the ordered and well-defined PdZn pairs provide a dual-site geometric structure conducive to the key C-N coupling with a low kinetical barrier,as demonstrated on both operando measurements and theoretical calculations.Consequently,the PdZn electrocatalyst displays excellent performance for the co-reduction to generate urea with a maximum urea Faradaic efficiency of 62.78%and a urea yield rate of 1274.42μg mg^(-1) h^(-1),and the latter is 1.5-fold larger than disordered pairs in PdZn alloys.This work paves new pathways to boost urea electrosynthesis via constructing ordered dual-metal pairs.

关 键 词：Electrochemical C-N coupling Urea electrosynthesis Intermetallic compounds Geometric structures Active pairs 

分 类 号：TQ441.41[化学工程—化学肥料工业]