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

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

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Electric double layer(EDL)is a critical topic in electrochemistry and largely determines the working per-formance 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 elec-trochemical 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 N-doped 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.

Lithium batteriesGraphiteN-dopingElectric double layerMolecular dynamicsConstant potential methodElectrode potential

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

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Tsinghua Center for Green Chemical Engineering Electrification(CCEE),Department of Chemical Engineering,Tsinghua University,Beijing 100084,China

Beijing Advanced Innovation Center for Materials Genome Engineering Institute for Advanced Materials and Technology,University of Science and Technology Beijing,Beijing 100083,China

National Materials Corrosion and Protection Data Center,University of Science and Technology Beijing,Beijing 100083,China

Ordos Carbon Neutral Research and Application Co.,Ltd.,Ordos 017010,Inner Mongolia,China

Institute for Carbon Neutrality,Tsinghua University,Beijing 100084,China

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

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National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Key Research and Development ProgramOpen Research Fund of CNMGE Platform&NSCC-TJ,Ordos-Tsinghua Innovative & Collaborative Research Program in Carbon NeutralityTsinghua University Initiative Scientific Research Program

T23220152220909422209093221090862021YFB2500300

2024

10.1016/j.jechem.2024.01.058

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.93(6)
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