物理化学学报 >> 2026, Vol. 42 >> Issue (4): 100204.doi: 10.1016/j.actphy.2025.100204

所属专题： 二次电池先进正极材料

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缓解硫化物基全固态电池对压力的依赖性：高镍正极的结构与界面调控策略

张亚娟1,†, 黎晋良2,†, 张希1,*(), 李悦3, 孙鹏2, 徐昊4, 潘丽坤3,*()   

  1. 1 上海交通大学机械与动力工程学院, 上海 200240
    2 暨南大学物理与光电工程学院物理学系, 广东省真空镀膜技术与新能源材料工程技术研究中心, 思源实验室, 广东 广州 510632
    3 华东师范大学物理与电子科学学院, 上海磁共振重点实验室, 医学磁共振与分子影像技术研究院, 上海 200241
    4 Faculty of Chemistry and Food Chemistry & Center for Advancing Electronics Dresden, Technische Universit?t Dresden, Dresden 01062, Germany
  • 收稿日期:2025-07-21 修回日期:2025-09-08 录用日期:2025-10-20 发布日期:2026-01-29
  • 通讯作者: Email: braver1980@sjtu.edu.cn (张希)lkpan@phy.ecnu.edu.cn (潘丽坤)
  • 作者简介:

    †These authors contributed equally.

Mitigate pressure dependence in sulfide-based all-solid-state batteries via structural and interfacial engineering of Ni-rich cathodes

Yajuan Zhang1, Jinliang Li2, Xi Zhang1,*(), Yue Li3, Peng Sun2, Hao Xu4, Likun Pan3,*()   

  1. 1 School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
    2 Siyuan Laboratory, Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Department of Physics, College of Physics & Optoelectronic Engineering, Jinan University, Guangzhou 510632, Guangdong Province, China
    3 Shanghai Key Laboratory of Magnetic Resonance, School of Physics and Electronic Science, Institute of Magnetic Resonance and Molecular Imaging in Medicine, East China Normal University, Shanghai 200241, China
    4 Faculty of Chemistry and Food Chemistry & Center for Advancing Electronics Dresden, Technische Universit?t Dresden, Dresden 01062, Germany
  • Received:2025-07-21 Revised:2025-09-08 Accepted:2025-10-20 Published:2026-01-29
  • Contact: Email: braver1980@sjtu.edu.cn (Xi Zhang)lkpan@phy.ecnu.edu.cn (Likun Pan)

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摘要：

基于硫化物的全固态锂离子电池因其高能量密度和固有安全性而被视为下一代储能技术。然而，其对外部堆叠压力的高度依赖带来了显著挑战，限制了能量效率、结构灵活性及实际应用。本文重点探讨实现低压力操作的关键问题，并系统总结应对这些限制的策略，包括正负极改性、界面工程、电解质优化及操作参数调控。对于高镍层状正极，通过精确控制颗粒尺寸、组成梯度掺杂、孔结构设计以及界面涂层可缓解压力引起的机械降解。优化颗粒尺寸分布和电极-电解质界面化学有助于提升离子传输速率和界面稳定性，而兼具机械柔性与黏附性的先进高分子粘结剂可增强复合电极的机械韧性。在系统层面，通过温度调控、电化学窗口优化及等静压力控制等策略，可进一步增强材料层优化的效果。最后，本文提出跨尺度设计框架，将材料内在工程、动态界面稳定及系统级控制整合，以实现低压或常压下的稳定电池性能，推动全固态锂离子电池从实验研究向实际应用的转化。

关键词: 全固态锂电池, 堆叠压力, 高镍正极, 界面稳定性

Abstract:

Sulfide-based all-solid-state lithium-ion batteries (ASSLIBs) have emerged as one of the most promising candidates for next-generation energy storage systems owing to their high energy density, wide electrochemical stability window, and intrinsic safety benefits over liquid electrolyte counterparts. Nevertheless, their practical implementation faces a fundamental bottleneck: the strong dependence on high external stack pressure to maintain interfacial contact and suppress mechanical degradation during operation. This requirement not only reduces energy efficiency and packaging flexibility but also severely restricts scalability and commercialization, as maintaining uniform high pressure in large-format cells is technically challenging and economically costly. Addressing the critical challenge of achieving low-pressure or even ambient-pressure operation in sulfide-based ASSLIBs is therefore of both scientific and technological significance. In this review, we systematically analyze the origins of pressure-dependent performance, including particle fracture in Ni-rich layered cathodes, dynamic interfacial instability, and insufficient mechanical compliance of composite electrodes. Building on this mechanistic understanding, we summarize recent advances and design strategies across multiple scales. At the cathode level, particle size regulation, compositional doping, and engineered porosity, combined with conformal interfacial coatings, effectively mitigate stress concentration and suppress degradation. On the electrolyte and electrode interface, optimizing particle size distribution, tailoring interfacial chemistry, and introducing dynamic polymeric binders with balanced adhesion and elasticity significantly enhance ionic transport and maintain robust contact under low pressure. At the system level, strategies such as optimized temperature management, adjustment of the electrochemical window, and controlled isostatic pressure provide additional means to stabilize operation and complement materials-level solutions. Taken together, these advances demonstrate that the key to pressure-independent ASSLIBs lies in a synergistic design framework that integrates intrinsic materials engineering, interfacial stabilization, and system-level control. We further propose a cross-scale design roadmap toward the realization of low-pressure and flexible ASSLIBs, highlighting the need for dynamic adaptation between mechanical properties and electrochemical processes. This perspective underscores that enabling stable performance under minimized external pressure is not only essential for translating laboratory demonstrations into practical large-scale devices but also paves the way for safer, lighter, and more energy-efficient solid-state battery technologies.

Key words: All-solid-state lithium battery, Stack pressure, Ni-rich cathode, Interfacial stability