锂离子电池石墨负极包覆研究进展

doi:10.1016/j.actphy.2025.100096

物理化学学报 >> 2025, Vol. 41 >> Issue (9): 100096.doi: 10.1016/j.actphy.2025.100096

锂离子电池石墨负极包覆研究进展

祝鑫彤¹^,², 曹斌²^,³, 闫崇⁴, 唐城²^,⁵^,*(), 陈爱兵¹^,*(), 张强²^,⁶^,*()

¹ 河北科技大学化学与制药工程学院, 石家庄 050018
² 清华大学化学工程系, 复合固态电池北京市重点实验室, 清华大学绿电化工研究中心, 北京 100084
³ 西安科技大学材料科学与工程学院, 西安 710054
⁴ 北京理工大学前沿交叉科学研究院, 北京 100081
⁵ 鄂尔多斯实验室, 内蒙古鄂尔多斯 017000
⁶ 清华大学碳中和研究院, 北京 100084

收稿日期:2025-03-05 修回日期:2025-04-11 录用日期:2025-04-18 发布日期:2025-07-04
通讯作者: Email: cheng–net0@tsinghua.edu.cn (唐城)chen_ab@163.com (陈爱兵)zhang–qiang@mails.tsinghua.edu.cn (张强)
基金资助:
国家重点研发计划(2022YFB2404402); 华能集团总部科技项目基础能源科技研究专项(四)(HNKJ23–H71); 国家自然科学基金(22478221); 国家自然科学基金(U23A20573); 国家自然科学基金(U23A20140); 河北省自然科学基金(B2024208091); 河北省省级科技计划(22344402D); 清华大学自主科研项目

Advances in coating strategies for graphite anodes in lithium-ion batteries

Xintong Zhu¹^,², Bin Cao²^,³, Chong Yan⁴, Cheng Tang²^,⁵^,*(), Aibing Chen¹^,*(), Qiang Zhang²^,⁶^,*()

¹ College of Chemical and Pharmaceutical Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, China
² Beijing Key Laboratory of Complex Solid State Batteries & Tsinghua Center for Green Chemical Engineering Electrification, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
³ College of Materials Science and Engineering, Xi'an University of Science and Technology, Xi'an 710054, China
⁴ Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, China
⁵ Ordos Laboratory, Ordos 017000, Inner Mongolia Autonomous Region, China
⁶ Institute for Carbon Neutrality, Tsinghua University, Beijing 100084, China

Received:2025-03-05 Revised:2025-04-11 Accepted:2025-04-18 Published:2025-07-04
Contact: Email: cheng–net0@tsinghua.edu.cn (Cheng Tang)chen_ab@163.com (Aibing Chen)zhang–qiang@mails.tsinghua.edu.cn (Qiang Zhang)
Supported by:
the National Key Research and Development Program of China(2022YFB2404402); Huaneng Group science and technology research project(HNKJ23–H71); National Natural Science Foundation of China(22478221); National Natural Science Foundation of China(U23A20573); National Natural Science Foundation of China(U23A20140); the Hebei Natural Science Foundation(B2024208091); S&T Program of Hebei(22344402D); Tsinghua University Initiative Scientific Research Program

摘要/Abstract

摘要：

石墨负极是目前锂离子电池中广泛使用的商品化负极材料，其在接触电解液发生储锂时会因有机电解液的还原分解而形成一层固体电解质界面膜(SEI)。该界面膜对锂离子电池的循环稳定性、快充性能、安全性能等诸多方面有着关键影响。通过在石墨表面构建一层包覆层，减少其与电解液之间的副反应并促进稳定电极界面的形成，可以提高储锂的电化学性能。表面包覆通常通过气相或液相法实现，包覆材料主要包括碳材料、锂离子导体、金属化合物和聚合物材料等体系。本文评述了不同包覆材料和方法对石墨负极性能的提升作用，分析了包覆改性策略影响电池快充性能和循环稳定性的机制，为锂离子电池负极材料的研究和开发提供了材料物理化学基础。

关键词: 石墨负极, 碳负极, 表面包覆, 固体电解质界面膜, 锂离子电池

Abstract:

As a critical component for achieving sustainable energy systems, secondary lithium-ion batteries (LIBs) have become the dominant electrochemical energy storage technology. Graphite has been widely employed as an anode material in rechargeable LIBs, where the formation of a solid electrolyte interphase (SEI) on graphite particles plays a pivotal role in realizing optimal Li⁺ ion storage performance. However, solvent co-intercalation with Li⁺ ions leads to volumetric expansion, unstable SEI formation, irreversible capacity loss, structural layer collapse, and even lithium dendrite formation. To overcome these challenges, surface coating modification has emerged as an effective strategy to enhance graphite anode performance. This review systematically summarizes recent progress in coating materials (including carbon materials, lithium-ion conductors, metal compounds, and polymers) fabricated through vapor-phase or liquid-phase deposition. Enormous research investigations demonstrate that rationally designed coating layers prevent direct electrolyte/graphite contact to inhibit solvent decomposition, regulate lithium-ion flux distribution to promote uniform deposition, and function as artificial SEI components to improve interphasial stability. This review provides both theoretical insights and practical considerations for future research and development of advanced graphite anode materials for lithium-ion batteries.

Key words: Graphite anode, Carbon anode, Surface coating, Solid-electrolyte interphase, Lithium-ion battery

祝鑫彤, 曹斌, 闫崇, 唐城, 陈爱兵, 张强. 锂离子电池石墨负极包覆研究进展[J]. 物理化学学报, 2025, 41(9), 100096. doi: 10.1016/j.actphy.2025.100096

Xintong Zhu, Bin Cao, Chong Yan, Cheng Tang, Aibing Chen, Qiang Zhang. Advances in coating strategies for graphite anodes in lithium-ion batteries[J]. Acta Phys. -Chim. Sin. 2025, 41(9), 100096. doi: 10.1016/j.actphy.2025.100096

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100096

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I9/100096

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Coating method	Coating layer homogeneity	Cost	Complexity of process	Temperature/Pressure	Applicable coating materials
Hydrothermal	High	High	Simple process, not optimized for large-scale application	Medium temperature, high pressure	Carbon material, Li-ion conductor, metal compound
Co-precipitation	Medium	Low	Mature process, scalable for large-scale application	Room temperature	Carbon material, Li-ion conductor, metal compound
Sol-gel	High	Low	Mature process, scalable for large-scale application	Room temperature	Carbon material, Li-ion conductor, metal compound, polymer material
Chemical vapor deposition	High	Medium	Mature process, scalable for large-scale application	High temperature (> 500 ℃)	Carbon material, Li-ion conductor, metal compound, polymer material
Atomic/molecular layer deposition	Extremely high	Extremely high	Complex process, not optimized for large-scale application	Medium temperature	Carbon material, Li-ion conductor, metal compound
Spray drying	High	Medium	Mature process, scalable for large-scale application	Medium temperature	Carbon material, Li-ion conductor, metal compound

Coating material	Key features	Ionic conductivity	Electrical conductivity	SEI regulation/mechanical properties	Electrochemical properties
Carbon material	Conductive for both ions and electrons	Large interlamellar spacing promotes Li⁺ diffusion	High conduction	Thin and stable SEl formation/low hardness	Improve the initial Coulombic efficiency and rate performance
Li-ion conductor	High conductivity of Li⁺ ions	Accelerating desolvation	Insulation	Inorganic-rich SEI/medium hardness	Improve the low-temperature and fast-charging performance
Metal compound	Electrically conductive, stable interface	High Li⁺ adsorption	Insulation or partial conduction	Physically hinder electrolyte decomposition/high hardness	Improve the cycle stability
Polymer material	Flexible SEI, uniform deposition of Li	Polar groups promote Li⁺ conduction	Insulation or partial conduction	Inner organic-outer inorganic composite SEI/high flexibility	Reduce lithium dendrites

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锂离子电池石墨负极包覆研究进展

Advances in coating strategies for graphite anodes in lithium-ion batteries

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