Work-function effect of Ti_(3)C_(2)/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage  

作　　者：Huicong Xia Lingxing Zan Hongliang Dong Yifan Wei Yue Yu Jinfu Shu Jia-Nan Zhang Chong-Xin Shan 

机构地区：[1]Key Laboratory of Advanced Energy Catalytic and Functional Material Preparation of Zhengzhou,College of Materials Science and Engineering,Zhengzhou University,Zhengzhou 450001,China [2]Key Laboratory of Materials Physics of Ministry of Education,School of Physics and Microelectronics,Zhengzhou University,Zhengzhou 450001,China [3]Key Laboratory of Chemical Reaction Engineering of Shaanxi Province,College of Chemistry and Chemical Engineering,Yan’an University,Yan’an 716000,China [4]Center for High Pressure Science and Technology Advanced Research,Pudong,Shanghai 201203,China [5]Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University,Tianjin 300071,China

出　　处：《Nano Research》2024年第8期7163-7173,共11页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.U22A20107,22162026,and 42050203);the Science and Technology Research and Develpoment Program Joint Fund Project of Henan Provincial(No.222301420001);the Distinguished Young Scholars Innovation Team of Zhengzhou University(No.32320275);Key Research Projects of University in Henan Province(No.24A150041);Henan Province Science and Technology Research Projects(No.242102240106);Postdoctoral Fellowship Program of CPSF(No.GZC20232382).

摘　　要：In the quest to enhance the efficiency of sodium-ion batteries,the dynamics of solid electrolyte interphase(SEI)formation are of paramount importance.The SEI layer’s integrity is integral to the charge–discharge efficiency and the overall longevity of the battery.Herein,a novel two-dimensional Ti_(3)C_(2) fragments enmeshed on iron-nitrogen-carbon(Fe-N-C)nanosheets(Ti_(3)C_(2)/Fe-NC)has been synthesized.This electrode features a matrix which has been shown to expedite SEI layer formation through the facilitation of selective anion adsorption,thus augmenting battery performance.Density functional theory calculation reveals that the SEI evolution energy of NaPF6 at the Ti_(3)C_(2)/Fe-N-C interface is 0.81 eV,significantly lower than the Ti_(3)C_(2)(1.23 eV).This process is driven by the electron transportation from Ti_(3)C_(2) to Fe-N-C substrate,facilitated by their work-function difference,leading to the formation of ferromagnetic Fe species,which possesses Fe 3d d_(xz)d_(z)2 orbitals and undergoes hybridization with theπandσorbitals of NaF,creating a key intermediate during charging.This process diminishes the antibonding energy and attenuates the orbital interaction with NaF,thus reducing the activation energy and improving the SEI formation reaction kinetics.Consequently,it leads to the creation of multi-interface SEI characterized by high-throughput ion transport and an efficient reaction network.

关 键 词：Ti_(3)C_(2)/Fe-N-C heterostructure WORK-FUNCTION electron interaction solid electrolyte interphase sodium storage 

分 类 号：TM912[电气工程—电力电子与电力传动]