Probing the electric double layer structure at nitrogen-doped graphite electrodes by constant-potential molecular dynamics simulations  

作　　者：Legeng Yu Nan Yao Yu-Chen Gao Zhong-Heng Fu Bo Jiang Ruiping Li Cheng Tang Xiang Chen 

机构地区：[1]Tsinghua Center for Green Chemical Engineering Electrification(CCEE),Department of Chemical Engineering,Tsinghua University,Beijing 100084,China [2]Beijing Advanced Innovation Center for Materials Genome Engineering,Institute for Advanced Materials and Technology,University of Science and Technology Beijing,Beijing 100083,China [3]National Materials Corrosion and Protection Data Center,University of Science and Technology Beijing,Beijing 100083,China [4]Ordos Carbon Neutral Research and Application Co.,Ltd.,Ordos 017010,Inner Mongoli1,China [5]Institute for Carbon Neutrality,Tsinghua University,Beijing 100084,China [6]Center for Next-Generation Energy Materials and School of Chemical Engineering,Sungkyunkwan University,2066 Seobu-ro,Jangan-gu,Suwon-si,Gyeonggi-do 16419,Republic of Korea

出　　处：《Journal of Energy Chemistry》2024年第6期299-305,I0008,共8页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(T2322015,22209094,22209093,and 22109086);the National Key Research and Development Program(2021YFB2500300);the Open Research Fund of CNMGE Platform&NSCC-TJ;Ordos-Tsinghua Innovative&Collaborative Research Program in Carbon Neutrality;the Tsinghua University Initiative Scientific Research Program。

摘　　要：Electric double layer(EDL)is a critical topic in electrochemistry and largely determines the working performance of lithium batteries.However,atomic insights into the EDL structures on heteroatom-modified graphite anodes and EDL evolution with electrode potential are very lacking.Herein,a constant-potential molecular dynamics(CPMD)method is proposed to probe the EDL structure under working conditions,taking N-doped graphite electrodes and carbonate electrolytes as an example.An interface model was developed,incorporating the electrode potential and atom electronegativities.As a result,an insightful atomic scenario for the EDL structure under varied electrode potentials has been established,which unveils the important role of doping sites in regulating both the EDL structures and the following electrochemical reactions at the atomic level.Specifically,the negatively charged N atoms repel the anions and adsorb Li~+at high and low potentials,respectively.Such preferential adsorption suggests that Ndoped graphite can promote Li~+desolvation and regulate the location of Li~+deposition.This CPMD method not only unveils the mysterious function of N-doping from the viewpoint of EDL at the atomic level but also applies to probe the interfacial structure on other complicated electrodes.

关 键 词：Lithium batteries Graphite N-DOPING Electric double layer Molecular dynamics Constant potential method Electrode potential 

分 类 号：O646[理学—物理化学] TM912[理学—化学]