石墨烯基双原子催化剂电催化氮还原氨的理论研究  

Theoretical study on electrocatalytic reduction of nitrogen to ammonia by graphene-based diatomic catalyst

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)

机构地区：[1]河北科技工程职业技术大学资源与环境工程系,河北邢台054000

出　　处：《化学研究与应用》2025年第3期669-676,共8页Chemical Research and Application

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.

关 键 词：密度泛函理论 氮还原反应 双原子催化剂 石墨烯 

分 类 号：O612.4[理学—无机化学]