1. 西南交通大学 智慧城市与交通学院，四川 成都 611756；2. 西南交通大学 电气工程学院，四川 成都 611756
张海涛，吴阳晨. 固态电解质与粉体电极界面的基础问题及优化策略［J］. 中国粉体技术，2025，31（5）：1-17.
ZHANG Haitao， WU Yangchen. Fundamental issues and optimization strategies of solid-state electrolyte-powder electrode interface［J］. China Powder Science and Technology，2025，31（5）：1−17.
DOI：10.13732/j.issn.1008-5548.2025.05.003
收稿日期：2024-11-13，修回日期：2025-06-06，上线日期：2025-06-28。
基金项目：国家自然科学基金项目，编号：52477224，51977185；四川省自然科学基金项目，编号：2023NSFSC0441。
第一作者简介：张海涛（1985），男，特聘研究员，博士，博士生导师，四川省学术和技术带头人后备人选，研究方向为电化学储能。E-mail：haitaozhang@swjtu. edu. cn。
摘要：【目的】 为了解决固态电解质与粉体电极界面兼容性问题，综述固态电解质与粉体电极界面的基础问题及优化策略，为固态电池的进一步研究与发展提供参考。【研究现状】 概述固态电解质与电极界面的基础理论并分析界面弱连接、界面稳定性以及界面离子传导受阻等界面问题；详细介绍相场模拟技术、有限元仿真技术和第一性原理计算等电极材料与电解质界面性能优化模拟技术；探讨电极材料与电解质界面问题的改性策略，包括界面接触的增强和界面稳定性的提升，剖析电场内电荷行为对界面稳定性的影响。【结论与展望】提出当前固态电池在发展进程中面临着诸多严峻挑战，认为界面性能优化策略对解决固态电解质与粉体电极界面的基础问题至关重要，实施这些策略有望突破固态电池的发展瓶颈。
关键词：固态电解质；粉体电极；界面问题；优化策略；模拟技术
Significance The dual-carbon goals have spurred a significant shift in the industry, accelerating transformation and imposing higher requirements on lithium battery technologies. Driven by innovations in downstream applications, the demand for lithium batteries with higher energy density and enhanced safety has increased. Traditional liquid batteries utilizing flammable organic electrolytes are susceptible to thermal runaway, which may trigger chain reactions leading to battery pack failure and increased fire risks. Consequently, solid-state battery technology has emerged as an innovative solution, garnering growing research attention. By replacing flammable liquid electrolytes with solid-state alternatives, these batteries inherently mitigate the risks of fire and explosion while significantly improving safety performance. Moreover, solid-state batteries effectively suppress dendrite formation, thereby substantially enhancing energy density, stability, and reliability. Despite significant progress in developing highly conductive solid-state electrolytes, most all-solid-state batteries still suffer from constrained rate performance, primarily attributed to the interfacial impedance at the solid-state electrolyte-electrode interface. However, the precise mechanisms governing this impedance remain experimentally elusive. Optimizing the solid electrolyte-powder electrode interface continues to be one of the pivotal challenges in propelling its commercialization.
Progress In recent years, significant breakthroughs have been made in solid-state electrolyte-electrode interface research, with the focus evolving from basic theoretical exploration to addressing key scientific challenges. Based on fundamental principles，three interface types were investigated theoretically. The inherent causes for poor interfacial contact, stability issues, and impeded ionic conduction were analyzed. Moreover, the intrinsic connection between interfacial contact resistance, electrochemical stability, and ionic transport kinetics was systematically elucidated, thereby laying a solid foundation for interfacial optimization. Methodologically, advanced simulation techniques have emerged as powerful tools for investigating interfacial phenomena and predicting material behaviors. Phase-field simulations were used to model both interfacial layer formation and electrolyte microstructure evolution. Finite element analysis was used to quantitatively characterize the interface thermal behavior and stress distribution. This combined approach provides multidimensional insights into the anisotropic characteristics of lithium dendrite growth. In addition, finite element simulation was used to model battery aging processes during solid-state battery development. First-principles calculations haven proven particularly valuable for studying interfacial charge transfer mechanisms and reaction kinetics, while density functional theory (DFT) provided an efficient approach to predicting the electrode-electrolyte interfacial reactions. Nevertheless, limitations persist in accurately simulating dynamic contact behaviors at complex powder/porous-electrolyte interfaces. To address these interfacial challenges, several innovative strategies were proposed. The introduction of transition interlayers reduced interface resistance and enhanced cycle stability by increasing interfacial contact. Structural optimization strategies, particularly through sandwich configurations and three-dimensional architectures, have emerged as a promising research direction for enhancing interfacial contact. Furthermore, interfacial engineering through buffer layer design and stabilizer incorporation enhanced electrolyte-electrode interface contact, thereby improving solid-state battery performance. Additionally, a comprehensive understanding of charge behaviors under electric fields is considered crucial for achieving stable interfaces.
Conclusions and Prospects Despite the progress achieved in solid-state lithium battery technology, several critical challenges must be overcome to realize its widespread adoption in energy storage systems. These challenges are intricate and multifaceted, with interfacial phenomena representing a particularly complex aspect that requires comprehensive consideration during design and optimization. Both chemical-electrochemical and physical factors must be taken into account, with special emphasis on understanding the physical interface through detailed analysis and refinement of cell internal architecture. Although simulation techniques provide theoretical support for interface optimization, their practical implementation still faces significant limitations. In addition, the development of advanced characterization techniques is essential for clarifying the correlations between electrochemical performance degradation and the electrode-electrolyte interface. These techniques can shed light on the microscopic changes at the interface and thus provide a scientific basis for improving the interfacial performance.
Keywords：solid-state electrolyte; powder electrode; interfacial issues; optimization strategy; simulation technique
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