Unraveling Lithium-Ion Transport in Solid Electrolyte Interphase: from Composition to Interface Dynamics via Molecular Dynamics Simulations

Qianqian Wang; Tairan Wang; Pu Zhang; Deshuai Yang; Cuili Zhang; Lang Wang; Shengbo Lu; Tracy Chenmin Liu; Shihan Qi; Weiguo Huang; Jingjing Liu; Guannan Zhu; Jun Fan

doi:10.1002/smll.202503340

Unraveling Lithium-Ion Transport in Solid Electrolyte Interphase: from Composition to Interface Dynamics via Molecular Dynamics Simulations

Qianqian Wang (Co-first Author)
, Tairan Wang (Co-first Author)
, Pu Zhang
, Deshuai Yang
, Cuili Zhang
, Lang Wang
, Shengbo Lu
, Tracy Chenmin Liu
, Shihan Qi
, Weiguo Huang
, Jingjing Liu
, Guannan Zhu^*
, Jun Fan^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

5 Citations (Scopus)

4 Downloads (CityUHK Scholars)

Abstract

Lithium-ion transport across the solid electrolyte interphase (SEI) is a key procedure in charging which determines the performance and stability of lithium-ion batteries (LIBs). However, an atomic-level understanding of the overall transport process from electrolyte through SEI remains elusive, particularly regarding the thermodynamic and kinetic parameters that govern this cross-interface phenomenon. In this study, molecular dynamics (MD) simulations are employed to systematically investigate the complete Li-ion transport progress, encompassing the electrolyte, organic/inorganic SEI components, and two critical interfaces: electrolyte/organic SEI and organic SEI/inorganic SEI. The results indicate that Li ions in the organic SEI retain either full or partial solvation shells. Free energy profiles reveal that the highest energy barrier emerges at the organic–inorganic SEI interface due to the complete desolvation of Li ions and structural differences between the organic and inorganic SEI layers. By constructing a comprehensive free energy landscape for Li-ion transport, this study offers valuable insights into the relationship between SEI composition, structure, and interfacial dynamics.

© 2025 Wiley-VCH GmbH

Original language	English
Article number	2503340
Number of pages	7
Journal	Small
Volume	21
Issue number	31
Online published	4 Jun 2025
DOIs	https://doi.org/10.1002/smll.202503340
Publication status	Published - 7 Aug 2025

Funding

This work was supported by the Hong Kong Research Grant Council Collaborative Research Fund: C1002-21G and C1017-22G, as well as City University of Hong Kong Project no. 7006111 and ITC project ITP/034/23NP.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

energy barrier
Li-ion transport
lithium-ion batteries
molecular dynamics simulation
solid electrolyte interphase

Publisher's Copyright Statement

This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

RGC Funding Information

RGC-funded

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10.1002/smll.202503340

298008902.pdfFinal Published version, 3.17 MBLicence: CC BY

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@article{a2ced8cc334d49dbaf1f4af806b5a923,

title = "Unraveling Lithium-Ion Transport in Solid Electrolyte Interphase: from Composition to Interface Dynamics via Molecular Dynamics Simulations",

abstract = "Lithium-ion transport across the solid electrolyte interphase (SEI) is a key procedure in charging which determines the performance and stability of lithium-ion batteries (LIBs). However, an atomic-level understanding of the overall transport process from electrolyte through SEI remains elusive, particularly regarding the thermodynamic and kinetic parameters that govern this cross-interface phenomenon. In this study, molecular dynamics (MD) simulations are employed to systematically investigate the complete Li-ion transport progress, encompassing the electrolyte, organic/inorganic SEI components, and two critical interfaces: electrolyte/organic SEI and organic SEI/inorganic SEI. The results indicate that Li ions in the organic SEI retain either full or partial solvation shells. Free energy profiles reveal that the highest energy barrier emerges at the organic–inorganic SEI interface due to the complete desolvation of Li ions and structural differences between the organic and inorganic SEI layers. By constructing a comprehensive free energy landscape for Li-ion transport, this study offers valuable insights into the relationship between SEI composition, structure, and interfacial dynamics. {\textcopyright} 2025 Wiley-VCH GmbH",

keywords = "energy barrier, Li-ion transport, lithium-ion batteries, molecular dynamics simulation, solid electrolyte interphase",

author = "Qianqian Wang and Tairan Wang and Pu Zhang and Deshuai Yang and Cuili Zhang and Lang Wang and Shengbo Lu and Liu, \{Tracy Chenmin\} and Shihan Qi and Weiguo Huang and Jingjing Liu and Guannan Zhu and Jun Fan",

year = "2025",

month = aug,

day = "7",

doi = "10.1002/smll.202503340",

language = "English",

volume = "21",

journal = "Small",

issn = "1613-6810",

publisher = "Wiley-VCH Verlag GmbH",

number = "31",

}

Unraveling Lithium-Ion Transport in Solid Electrolyte Interphase: from Composition to Interface Dynamics via Molecular Dynamics Simulations. / Wang, Qianqian (Co-first Author); Wang, Tairan (Co-first Author); Zhang, Pu et al.
In: Small, Vol. 21, No. 31, 2503340, 07.08.2025.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Unraveling Lithium-Ion Transport in Solid Electrolyte Interphase

T2 - from Composition to Interface Dynamics via Molecular Dynamics Simulations

AU - Wang, Qianqian

AU - Wang, Tairan

AU - Zhang, Pu

AU - Yang, Deshuai

AU - Zhang, Cuili

AU - Wang, Lang

AU - Lu, Shengbo

AU - Liu, Tracy Chenmin

AU - Qi, Shihan

AU - Huang, Weiguo

AU - Liu, Jingjing

AU - Zhu, Guannan

AU - Fan, Jun

PY - 2025/8/7

Y1 - 2025/8/7

N2 - Lithium-ion transport across the solid electrolyte interphase (SEI) is a key procedure in charging which determines the performance and stability of lithium-ion batteries (LIBs). However, an atomic-level understanding of the overall transport process from electrolyte through SEI remains elusive, particularly regarding the thermodynamic and kinetic parameters that govern this cross-interface phenomenon. In this study, molecular dynamics (MD) simulations are employed to systematically investigate the complete Li-ion transport progress, encompassing the electrolyte, organic/inorganic SEI components, and two critical interfaces: electrolyte/organic SEI and organic SEI/inorganic SEI. The results indicate that Li ions in the organic SEI retain either full or partial solvation shells. Free energy profiles reveal that the highest energy barrier emerges at the organic–inorganic SEI interface due to the complete desolvation of Li ions and structural differences between the organic and inorganic SEI layers. By constructing a comprehensive free energy landscape for Li-ion transport, this study offers valuable insights into the relationship between SEI composition, structure, and interfacial dynamics. © 2025 Wiley-VCH GmbH

AB - Lithium-ion transport across the solid electrolyte interphase (SEI) is a key procedure in charging which determines the performance and stability of lithium-ion batteries (LIBs). However, an atomic-level understanding of the overall transport process from electrolyte through SEI remains elusive, particularly regarding the thermodynamic and kinetic parameters that govern this cross-interface phenomenon. In this study, molecular dynamics (MD) simulations are employed to systematically investigate the complete Li-ion transport progress, encompassing the electrolyte, organic/inorganic SEI components, and two critical interfaces: electrolyte/organic SEI and organic SEI/inorganic SEI. The results indicate that Li ions in the organic SEI retain either full or partial solvation shells. Free energy profiles reveal that the highest energy barrier emerges at the organic–inorganic SEI interface due to the complete desolvation of Li ions and structural differences between the organic and inorganic SEI layers. By constructing a comprehensive free energy landscape for Li-ion transport, this study offers valuable insights into the relationship between SEI composition, structure, and interfacial dynamics. © 2025 Wiley-VCH GmbH

KW - energy barrier

KW - Li-ion transport

KW - lithium-ion batteries

KW - molecular dynamics simulation

KW - solid electrolyte interphase

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DO - 10.1002/smll.202503340

M3 - RGC 21 - Publication in refereed journal

SN - 1613-6810

VL - 21

JO - Small

JF - Small

IS - 31

M1 - 2503340

ER -

Unraveling Lithium-Ion Transport in Solid Electrolyte Interphase: from Composition to Interface Dynamics via Molecular Dynamics Simulations

Abstract

Funding

UN SDGs

Research Keywords

Publisher's Copyright Statement

RGC Funding Information

Access Output

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Permanent Link

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ITF-ExtU-Lead: Development of High-Temperature Stable Electrolytes in Silicon-Based Batteries through Computational-assisted Design

CRF: Fundamental Study Towards Real Spider Dragline Silk Performance Through Artificial Innovative Approach

CRF: Aqueous Zn-based Batteries with Ultimate Safety and High Energy Density for Large Scale Energy Storage System

Cite this

Unraveling Lithium-Ion Transport in Solid Electrolyte Interphase: from Composition to Interface Dynamics via Molecular Dynamics Simulations

Abstract

Funding

UN SDGs

Research Keywords

Publisher's Copyright Statement

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Projects

ITF-ExtU-Lead: Development of High-Temperature Stable Electrolytes in Silicon-Based Batteries through Computational-assisted Design

CRF: Fundamental Study Towards Real Spider Dragline Silk Performance Through Artificial Innovative Approach

CRF: Aqueous Zn-based Batteries with Ultimate Safety and High Energy Density for Large Scale Energy Storage System

Cite this