摘要
氨是一种重要的能源物质,广泛地应用于人类的生产生活,但是目前生产氨的主要方法还是能源消耗量大,生产成本高的Haber-Bosch工艺,因此开发一种新型生产氨的工艺势在必行。电催化还原N_(2)合成氨被认为是最有希望替代传统工艺的生产方法。本文通过理论计算,通过构建石墨烯基双原子催化剂M_(2)/Gr(M=Mn,Fe,Co,Ni)研究了N2在其表面的吸附及还原特性。理论分析表明,N_(2)在Fe_(2)/Gr催化剂上还原为NH3的决速步能垒仅为0.69 eV,且氮还原反应(Nitrogen reduction reaction,NRR)的主要竞争反应析氢反应(Hydrogen evolution reactions,HER)的能垒为1.95 eV,证明Fe_(2)/Gr是一种高效、有选择性的电催化合成氨催化剂。
Ammonia is an important energy substance widely used in human production and life.However,the main method of producing ammonia currently is the Haber-Bosch process,which consumes a large amount of energy and has high production costs.Therefore,it is imperative to develop a new process for producing ammonia.Electrocatalytic nitrogen reduction reaction(NRR)to synthesize ammonia is considered the most promising production method to replace traditional processes.This article investigates the adsorption and reduction characteristics of N_(2)on the surface of graphene based diatomic catalysts M_(2)/Gr(M=Mn,Fe,Co,Ni)through theoretical calculations.Theoretical analysis shows that the rate determining step energy barrier for N_(2)reduction to NH_(3)on Fe_(2)/Gr catalyst is only 0.69 eV,and the energy barrier for the main competitive reaction hydrogen evolution reactions(HER)of NRR is 1.95 eV,proving that Fe_(2)/Gr is an efficient and selective electrocatalytic catalyst for ammonia synthesis.
作者
陈宁
田明
张志华
CHEN Ning;TIAN Ming;ZHANG Zhi-hua(Department of Resources and Environmental Engineering,Hebei Vocational University of Technology and Engineering,Xingtai 054000,China)
出处
《化学研究与应用》
北大核心
2025年第3期669-676,共8页
Chemical Research and Application
关键词
密度泛函理论
氮还原反应
双原子催化剂
石墨烯
density functional theory
nitrogen reduction reaction
diatomic catalyst
graphene
