A dual-site Fe-based catalyst for efficient ammonia synthesis under mild conditions  

作　　者：Shiyong Zhang Mingyuan Zhang Tianhua Zhang Jizhen Sun Jiaxin Li Kailin Su Ruishao Mao Yanliang Zhou Xuanbei Peng Yangyu Zhang Jun Ni Bingyu Lin Xiuyun Wang Lilong Jiang 

机构地区：[1]National Engineering Research Center of Chemical Fertilizer Catalyst,Fuzhou University,Fuzhou 350002,China [2]Qingyuan Innovation Laboratory,Quanzhou 362801,China

出　　处：《Science China Chemistry》2025年第4期1576-1584,共9页中国科学(化学英文版)

基　　金：supported by the National Key Research and Development Program of China(2021YFB4000400);the National Natural Science Foundation of China(22222801,22038002,92361303,22478075,22472028,and 22108037);the Key R&D Plan of Shanghai Science and Technology Commission(21DZ1209002).

摘　　要：Achieving green ammonia(NH_(3))synthesis requires developing effective catalysts under mild conditions.However;the competitive adsorption of N2 and H_(2);as well as the strong binding of N-containing intermediates on the catalyst;greatly inhibits the active sites for efficient NH_(3) synthesis.Here;we constructed a series of ZrH_(2)-modified Fe catalysts with dual active sites to address these issues and realized efficient NH_(3) synthesis under mild conditions.Our study shows that ZrH_(2) can not only provide active sites for H_(2) activation but also transfer electrons to Fe sites for accelerating N2 activation.The interaction between Fe and ZrH_(2) over 40ZrH_(2)-Fe leads to a decrease in work function and a downward shift of the d-band center;which is conducive to N2 activation and NH_(3) desorption;respectively.The utilization of distinct sites for activating different reactants can avoid the competitive adsorption of N2 and H_(2);leading to excellent NH_(3) synthesis activity of the 40 wt.%ZrH_(2)-mediated Fe catalyst.As a result;40ZrH_(2)-Fe exhibits a high NH_(3) synthesis rate of 23.3 mmol gcat-1h-1at 400℃and 1 MPa and robust stability during 100 h time-on-stream.

关 键 词：ammonia synthesis competitive adsorption dual-site catalyst N2 activation synergistic effect 

分 类 号：O643.36[理学—物理化学]