Dual-polymer engineered Ni-O-Si interface catalysts for selective and durable electrocatalytic urea synthesisOA
Nickel(Ni)is a promising catalyst for electrochemical urea oxidation reactions.However,its strong chemisorption of CO_(2) and the tendency for uncontrollable structural reconstruction during catalysis have limited the exploration of Ni-based catalysts in electrocatalytic urea synthesis.Herein,we propose a comodification strategy for Ni-mSiO_(x) using polydopamine(PDA)and polyethyleneimine(PEI)to enable efficient electrocatalytic co-reduction of nitrate and CO_(2) for urea synthesis.The incorporation of stable Ni-O-Si active sites effectively balanced competing reaction pathways,while dual polymer modification optimized the surface electronic structure,promoted the formation of pyrrolic/pyridinic nitrogen species(ProN/PN,86.7%),and accelerated C-N coupling kinetics.The resulting PDA/PEI-Ni-mSiO_(x) catalyst achieved a urea production rate of 2513μg·h^(−1) ·mg_(cay)^(−1) ,a Faradaic efficiency of 28.6%,and a urea selectivity of 54.2%.Notably,the catalyst retained over 90%of its activity after 39 h of continuous operation,with no observable structural degradation following repeated cycling.This work presents a robust strategy for the rational design of high-performance,durable Ni-based catalysts for urea electrosynthesis and provides mechanistic insights into the structure-activity relationships at polymer-metal oxide interfaces.
Weize Chen;Hui Su;Xiaoping Chen;Xuan Zheng;Zehua Zou;Jing Tang;Maosheng Zhang;Qingxiang Wang;Yun Ling;Jian-Feng Li
Fujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,ChinaFujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,ChinaFujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,ChinaFujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,ChinaFujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,ChinaKey laboratory for analytical science of food safety and biology,Ministry of Education,College of Chemistry,Fuzhou University,Fuzhou 350116,ChinaFujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,ChinaFujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,ChinaFujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University,Tianjin 300071,ChinaFujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology,Fujian Provincial Key Laboratory of Pollution Monitoring and Control,College of Chemistry,Chemical Engineering and Environment,Minnan Normal University,Zhangzhou 363000,China College of Energy,College of Chemistry and Chemical Engineering,State Key Laboratory of Physical Chemistry of Solid Surfaces,iChEM,College of Material,Xiamen University,Xiamen 361005,China
化学化工
electrocatalytic synthesis of ureaNi-O-Si interfacespolymer-metal oxide interfacesC-N coupling
《Nano Research》 2026 (2)
P.321-330,10
supported by the National Natural Science Foundation of China(Nos.21872034,22021001,and 92472203)the Natural Science Foundation of Fujian Province(Nos.2025J01363,2024J01807,and 2025J01973)the Natural Science Foundation of Zhangzhou City(No.ZZ2024J16)the Eagle Project of Fujian Province.
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