文献类型：期刊文献

英文题名：Efficient Electrocatalytic Urea Formation from Gas Pollutants on Heteronuclear Dual-Metal Atom Anchored N-Doped Graphene

作者：Lu, Song[1];Ying, Jiadi[1];Liu, Tiancun[1];Xu, Jianqing[1];Wang, Yeqing[1];Guo, Min[1];Shen, Qi[1];Wu, Yong[2];Zhao, Yafei[3];Yu, Zhixin[1]

机构：[1]Shaoxing Univ, Inst New Energy, Sch Chem & Chem Engn, Shaoxing 312000, Zhejiang, Peoples R China;[2]Dalian Univ Technol, Sch Chem, Dalian 116024, Peoples R China;[3]Henan Univ Sci & Technol, Sch Phys & Engn, Luoyang 471023, Peoples R China

年份：2024

卷号：38

期号：13

起止页码：11936

外文期刊名：ENERGY & FUELS

收录：SCI-EXPANDED(收录号：WOS:001249628100001)、、EI(收录号：20242616301303)、Scopus(收录号：2-s2.0-85196549613)、WOS

基金：This work is supported by the starting grant of Shaoxing University, the National Natural Science Foundation of China (No. 22208220) and the Zhejiang Provincial Natural Science Foundation of China (No. LQ23B030005).

语种：英文

外文关键词：Binary alloys - Copper alloys - Density functional theory - Doping (additives) - Electrocatalysis - Electrocatalysts - Iron alloys - Metabolism - Reduction - Zinc alloys

外文摘要：The electrochemical synthesis of urea under mild conditions is considered a promising alternative to the harsh industrial Haber-Bosch process. However, the development of highly active and selective electrocatalysts remains a formidable challenge. In this study, a novel mechanism for urea synthesis on dual-atom catalysts (DACs) using two gas pollutants (NO and CO) is proposed based on density functional theory (DFT) calculations. It is found that urea can be synthesized through consecutive C-N coupling and hydrogenation steps on heteronuclear DACs, in which the stable adsorption of NO and CO on DACs significantly contributes to the excellent performance for urea formation. Notably, only CoZn, CoCu, and FeZn@N-6/C can continuously accept proton-electron and ultimately achieve urea formation, exhibiting low limiting potentials of -0.27, -0.30, and -0.60 V, respectively. Furthermore, it is also determined that an alternative mechanism is preferable on three DACs. Moreover, competitive hydrogen evolution reaction, as well as reductions of CO and NO reductions, can be effectively suppressed, thereby endowing high selectivity for urea generation. Importantly, this study not only advances a novel mechanism for urea production utilizing gas pollutants but also broadens the applicability of DACs in electrocatalysis.