硅酸盐学报

锂电池液固电解质负极界面特性比较及改进策略

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朱浩天 ¹ , 张硕卿 ¹ , 张海阔 ¹ , 马宝琛 ¹ , 陈龙 ¹^,² , 李如宏 ¹^,² , 范修林 ¹

硅酸盐学报 | 全固态电池发展专刊—综合评述 2025,53(6): 1714-1727

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硅酸盐学报 |全固态电池发展专刊—综合评述 2025 , 53 (6) : 1714 -1727

锂电池液固电解质负极界面特性比较及改进策略

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朱浩天¹, 张硕卿¹, 张海阔¹, 马宝琛¹, 陈龙¹^,², 李如宏¹^,², 范修林¹

作者信息

^1．浙江大学材料科学与工程学院，杭州 310058

^2．浙江大学杭州国际科创中心，杭州 311215

通讯作者:

范修林（1984—），男，博士，研究员；

李如宏（1992—），男，博士，研究员。

作者简介:

朱浩天（2001—），男，博士研究生。

Liquid and Solid-State Li Electrolyte Anode Interface Properties Comparison and Enhancement Strategies

Haotian ZHU¹, Shuoqing ZHANG¹, Haikuo ZHANG¹, Baochen MA¹, Long CHEN¹^,², Ruhong LI¹^,², Xiulin FAN¹

Affiliations

^1.Zhejiang University, Hangzhou 310058, China

^2.ZJU-Hangzhou Global Scientific and Technological Innovation Center, Hangzhou 311215, China

Corresponding Author:

FAN Xiulin (1984-), male, Ph.D., Professor. E-mail: xlfan@zju.edu.cn;

LI Ruhong (1992-), male, Ph.D., Professor. ruhong@zju.edu.cn

ZHU Haotian (2001-), male, Doctoral candidate. E-mail: zhuhaotian@zju.edu.cn

出版时间: 2025-06-20 doi: 10.14062/j.issn.0454-5648.20240830

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摘要

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随着高性能锂电池需求的增加，电解质的设计及其界面调控成为提升电池性能的关键因素，其中，电解质界面性质密切影响电池的性能。液态电解质中的固体电解质界面相在充放电过程中容易发生变化，进而影响电池的库仑效率和循环稳定性；某些固态电解质具有理论上较好的安全性而受到广泛关注，但相比液态电解质，其面临更复杂的界面稳定性、离子/电子导电性以及离子流均匀性等挑战。固态电解质与液态电解质在界面特性上的显著差异，导致两者在锂枝晶生长、界面阻抗、离子迁移等方面的表现大相径庭。本文重点分析液态与固态电解质负极界面的特性差异及目前的研究进展，并提出优化电解质界面稳定性与离子流均匀性的改进策略，期望为未来新型高安全锂电池的设计提供理论指导与实践方向。

关键词

液态电解质 / 固态电解质 / 负极界面 / 固体电解质界面相 / 离子流

Abstract

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With the rapid advancement of electric vehicles, energy storage systems, and consumer electronics, a demand for high-performance lithium-ion batteries (LIBs) is escalating. The electrolyte plays a pivotal role in affecting the battery performance, safety, and longevity. Liquid electrolytes, which are widely used in commercial LIBs, offer high ionic conductivity and ease of processing. However, solid electrolyte interphase (SEI) formed in liquid electrolyte systems degrades during repeated charge-discharge cycles, increasing impedance, reducing the Coulombic efficiency, and compromising cycling stability. In contrast, solid-state electrolytes, known for their potential to enhance battery safety, face some challenges such as lower ion conductivity, poor mechanical properties, and difficulties in maintaining stable electrode interfaces under operational conditions.

The electrolyte-electrode interface, particularly at anode, is crucial for lithium battery performance. Lithium dendrite growth is a primary concern as it can cause short circuits and battery failure. In liquid electrolyte systems, dendrite formation is accelerated by uneven ion flow, SEI instability, and excessive current density. Solid-state electrolytes, while promising in terms of theoretical safety, also face some challenges, i.e., slower ion conductivity at room temperature and poor interface stability with lithium metal anodes. A better understanding of these differences is crucial for advancing electrolyte design.

One of the key challenges for liquid electrolytes is to control SEI formation. The chemical composition and morphology of the SEI directly impact the battery performance. A thick or uneven SEI layer increases internal resistance and slows ion flow, thereby reducing the Coulombic efficiency and cycle stability. In solid-state systems, the solid-solid interface between the electrolyte and electrode material leads to a high interfacial resistance, restricting ion migration and affecting charge-discharge efficiency. Ion transport in solid-state electrolytes is also more uneven and slower, further compromising safety. While SEI formation in liquid electrolytes can suppress dendrite growth and promote uniform lithium deposition, solid-state electrolytes tend to exhibit a higher interfacial resistance, which accelerates dendrite growth and leads to short circuits. These distinct interface properties are the main cause of the performance gap between liquid and solid-state batteries.

Optimizing interface stability and ion flow uniformity in both liquid and solid-state electrolytes is essential for improving battery technology. In this review, the characteristics of the anode interface in both systems are compared, with a focus on lithium dendrite growth mechanisms. Some factors like ion conductivity, electrode-electrolyte interactions, and interface stability that affect electrochemical performance are mentioned. This review also analyzes strategies to optimize electrolyte interface stability and ion flow uniformity in both liquid-state and solid-state systems. Electrolyte design strategies based on ion flow regulation to enhance ion conductivity, reduce interfacial resistance, and ensure more uniform ion distribution are proposed. These strategies include the development of advanced electrolyte materials, interface engineering to improve ion transport, and the use of hybrid systems that combine the advantages of both liquid and solid electrolytes.

Summary and prospects

Solid-state and liquid-state electrolytes exhibit significant differences, particularly in ionic conductivity and interface stability. While liquid electrolytes with their higher fluidity can quickly respond to ion flow, they face some challenges such as flammability and side reactions at the interface, which compromise battery safety. Solid-state electrolytes with their theoretically higher safety have attracted significant attention, but their practical application is limited due to the problems such as bulk inhomogeneity leading to uneven ionic conductivity and unstable electrode interfaces. Moreover, the mechanical rigidity of solid materials results in poor interface contact and stress accumulation during cycling, which further degrades battery performance and reduces cycle life. Achieving uniform ion flow is crucial for the stable cycling and optimal performance of batteries. Optimizing the ion mobility between the electrolyte and electrode is essential for improving efficiency and extending cycle life, regardless of whether the electrolyte is solid or liquid. Design strategies based on ion flow regulation can enhance electrolyte ionic conductivity via optimizing microstructure, advancing interface engineering, and developing composite electrolyte systems. These strategies improve ion mobility, reduce interface impedance, and enhance the beneficial feedback of the interface, leading to better cycling performance and stability. In addition, the rapid growth of machine learning and big data technologies also presents a transformative opportunity for novel electrolyte materials development. Moving forward, as battery technology progresses, electrolyte optimization will focus on improving the ionic conductivity of the electrolytes themselves and optimizing the entire battery system. In commercial applications, reducing failure rates to minimal levels is essential where safety standards are extremely stringent. To meet this, enhancing the ion flow and interface stability of electrolytes will be crucial for developing high-safety, long-lifetime batteries. Moreover, integrating machine learning and big data into electrolyte optimization will drive breakthroughs in battery performance, supporting the commercialization of next-generation high-performance batteries.

Key words

liquid electrolyte / solid-state electrolyte / anode interface / solid electrolyte interphase / ion flow

引用本文

朱浩天, 张硕卿, 张海阔, 马宝琛, 陈龙, 李如宏, 范修林. 锂电池液固电解质负极界面特性比较及改进策略. 硅酸盐学报, 2025 , 53 (6) : 1714 -1727 . DOI: 10.14062/j.issn.0454-5648.20240830

Haotian ZHU, Shuoqing ZHANG, Haikuo ZHANG, Baochen MA, Long CHEN, Ruhong LI, Xiulin FAN. Liquid and Solid-State Li Electrolyte Anode Interface Properties Comparison and Enhancement Strategies[J]. Journal of the Chinese Ceramic Society, 2025 , 53 (6) : 1714 -1727 . DOI: 10.14062/j.issn.0454-5648.20240830

基金

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浙江省重点研发计划(2023C01128)
国家自然科学基金(U21A2081)
国家重点研发计划(2022YFE0206300)
浙江省自然科学基金(LR23B030002)
中央高校基本科研基金(226-2024-00075)
浙江大学“百人计划”

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2025年第53卷第6期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240830

接收时间：2024-12-26
首发时间：2026-10-22
出版时间：2025-06-20

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出版历史

收稿日期：2024-12-26
修回日期：2025-01-06

基金

浙江省重点研发计划(2023C01128)

国家自然科学基金(U21A2081)

国家重点研发计划(2022YFE0206300)

浙江省自然科学基金(LR23B030002)

中央高校基本科研基金(226-2024-00075)

浙江大学“百人计划”

作者信息

^1．浙江大学材料科学与工程学院，杭州 310058

^2．浙江大学杭州国际科创中心，杭州 311215

通讯作者:

范修林（1984—），男，博士，研究员；

李如宏（1992—），男，博士，研究员。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240830

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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