Electroreduction NO to NH_(3)over single metal atom anchored on pyrrole type defective graphene:A DFT study  

作　　者：Jiazhi Wang Kai Li Qi Hao Dongxue Liu Xinbo Zhang 

机构地区：[1]State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China [2]University of Science and Technology of China,Hefei 230026,China [3]Key Laboratory of Automobile Materials,Ministry of Education,Jilin University,Changchun 130022,China

出　　处：《Chinese Chemical Letters》2023年第5期571-575,共5页中国化学快报（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(Nos.21725103,52072362);National Key R&D Program of China(No.2021YFB4000401);Youth Innovation Promotion Association CAS(No.E1202002)。

摘　　要：Electrochemical is considered an attractive approach to recycling the pollution NO(NORR)and producing the valuable NH_(3),which could simultaneously solve the two challenging problems,i.e.,NO removal and NH_(3)synthesis.Current research efforts focus less on NORR due to the lack of effective catalysts.Herein,based on DFT calculation,we try to explore effective pyrrole-type TM-N_(4)(TM=V,Cr,Mn,Fe,Co,Ni,Cu,Ru,Rh,Ta)catalysts for achieving the direct NORR.Among the investigated systems,Fe-N_(4)exhibits excellent catalytic activity and high NH_(3)selectivity.Moreover,the free energy of adsorption of N*has been proposed as a descriptor to predict and screen the effective TM-N_(4)catalyst for NORR and the crystal orbital halmilton populations(COHP)is used to describe the intrinsic relationship between metal atoms and the adsorption free energy of N^(*)intermediate.This work has provided a theoretical picture of TM-N4catalyzing NO to NH_(3),which will establish guidelines for the rational design of NORR catalysts and other electrochemical reactions.

关 键 词：DFT calculation Pyrrole-type DESCRIPTOR NORR COHP 

分 类 号：X701[环境科学与工程—环境工程] TQ113.26[化学工程—无机化工] TQ426