Axial coordinated iron-nitrogen-carbon as efficient electrocatalysts for hydrogen evolution and oxygen redox reactions  

作　　者：Yanan Zhou Li Sheng Lanlan Chen Wenhua Zhang Jinlong Yang 

机构地区：[1]School of Material Science and Chemical Engineering,Institute of Mass Spectrometry,Ningbo University,Ningbo 315211,China [2]Department of Chemical Physics,University of Science and Technology of China,Hefei 230026,China [3]Department of Material Science and Engineering,University of Science and Technology of China,Hefei 230026,China [4]Hefei National Laboratory for Physical Sciences at the Microscale,CAS Key Laboratory of Materials for Energy Conversion and Synergetic Innovation Centre of Quantum Information and Quantum Physics,University of Science and Technology of China,Hefei 230026,China

出　　处：《Chinese Chemical Letters》2025年第1期637-642,共6页中国化学快报(英文版)

基　　金：supported by the National Natural Science Foundation of China(Nos.22102167 and U21A20317)。

摘　　要：Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.

关 键 词：Axial coordinated ligands DFT calculation Hydrogen evolution reaction Oxygen evolution reaction Oxygen reduction reaction 

分 类 号：O64[理学—物理化学]