In situ evolution of Sn/Cu_(2)O heterostructure catalysts for modulating selectivity in electrosynthesis of ammonia and urea  

作　　者：Yinan Zheng Yuxin Jia Qiuhan Cao Lei Li Xin Yu Shiqi Zeng Hu Yao Xiaohui Guo 

机构地区：[1]Key Lab of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education,College of Chemistry and Materials Science,Northwest University,Xi'an 710069,China [2]College of Chemistry and Materials Engineering,Bohai University,Jinzhou 121013,China

出　　处：《Nano Research》2025年第3期169-177,共9页纳米研究(英文版)

基　　金：supported by the Key Projects of Intergovernmental International Cooperation in Key R&D Programs of the Ministry of Science and Technology of China(No.2021YFE0115800);the National Science Funding Committee of China(No.U20A20250);the Programs of the Science and Technology of Yulin City(No.CXY-2023-ZX04);the funding support from Shccig-Qinling Program.

摘　　要：Electrocatalytic nitrate reduction reaction(NO_(3)−RR)and its coupling with CO_(2)could provide new sustainable pathways for the synthesis of ammonia and urea,respectively.However,their practical applications are hindered by the lack of catalysts with satisfied Faraday efficiency and yield.Herein,we report self-supported electrochemically reconstituted Sn/Cu_(2)O bifunctional catalysts for the efficient synthesis of ammonia and urea.In the NO_(3)−RR,Sn/Cu_(2)O-βcatalysts electrodeposited for 800 s provided an excellent ammonia yield of 0.496 mmol·h(−1)·cm^(−2)and Faraday efficiency of 98.5%.Besides,Sn/Cu_(2)O-αcatalysts electrodeposited for 400 s achieved the maximum Faraday efficiency of 13.5%and outstanding urea yield of 32.35μmol·h^(−1)·cm^(−2)in C-N coupling.Comprehensive analyses confirm that bi-selectivity to ammonia and urea synthesis could be achieved by modulating the chemical state of Cu in Sn/Cu_(2)O catalysts,these results are superior to most reported transition metal-based catalysts in synthesis of urea and/or ammonia.In situ Fourier transform infrared(FTIR)spectroscopy revealed that^(*)CONH_(2)intermediates are essential for urea synthesis.This work will provide a feasible strategy for the development of bifunctional electrocatalysts for efficient ammonia and urea synthesis.

关 键 词：ELECTROCATALYSIS NH_(3)synthesis urea synthesis Sn/Cu_(2)O SELECTIVITY 

分 类 号：O64[理学—物理化学]