基于硫化物全固态锂离子电池混合正极的研究进展

doi:10.11949/0438-1157.20251089

摘要/Abstract

摘要：

硫化物全固态电池（ASSBs）因其能量密度高、安全性好，而成为最具前景的下一代电池技术之一。然而其电化学性能仍不尽如人意，特别是在高压正极、高质量负载条件下，混合正极内部存在固-固界面副反应的问题，并引发包括空间电荷层、体积膨胀、电子/离子传输等一系列问题，进而影响全固态电池性能。本文概述了目前对硫化物电池混合正极改性的研究现状，总结了材料表面改性（界面工程）、电解质改性（材料工程）、电极掺杂改性（部件工程）以及电极结构工程的相关发展现状及应用优势，并为下一步基于硫化物电解质的全固态锂电池混合正极的研发方向提供了指导性建议。

关键词: 硫化物全固态电池, 混合正极, 界面工程, 材料工程, 部件工程, 电极结构工程

Abstract:

Sulfide-based all-solid-state batteries (ASSBs) are considered one of the most promising next-generation battery technologies due to their high energy density and enhanced safety. However, their electrochemical performance still falls short of expectations, particularly under high-voltage cathodes and high-mass-loading conditions. Issues such as side reactions at solid-solid interfaces within the composite cathode can lead to problems including space charge layer formation, volume expansion, and hindered electron/ion transport, thereby compromising the overall performance of ASSBs. This article provides an overview of the current research progress on modifying composite cathodes in sulfide-based ASSBs. It summarizes recent advances in material surface modification (interface engineering), electrolyte optimization (material engineering), electrode doping and modification (component engineering), and electrode structural engineering, highlighting their respective advantages and applications. Furthermore, it offers guidance for future research directions in the development of composite cathodes for sulfide-based all-solid-state lithium batteries.

Key words: sulfide all-solid-state batteries, composite cathode, interface engineering, material engineering, component engineering, electrode structural engineering

中图分类号:

TM 911

杨立鹏, 顾宇阳, 田十宇, 杨晓光. 基于硫化物全固态锂离子电池混合正极的研究进展[J]. 化工学报, DOI: 10.11949/0438-1157.20251089.

Lipeng YANG, Yuyang GU, Shiyu TIAN, Xiao-Guang YANG. Recent Advances in Hybrid Cathodes for Sulfide-Based All-Solid-State Lithium-Ion Batteries[J]. CIESC Journal, DOI: 10.11949/0438-1157.20251089.

图/表 18

图1 硫化物全固态电池混合正极中的各种问题以及改性策略

Fig.1 Issues and Modification Strategies in the Composite Cathode of Sulfide-Based All-Solid-State Batteries.

表1 活性材料界面改性种类、机理以及优缺点

Table 1 Types， Mechanisms， and Advantages/Disadvantages of Interface Modification for Active Materials

改性策略/涂层类型		核心机理	优点	局限性	代表性文章
传统氧化物涂层	Li₄Ti₅O₁₂	在活性材料与硫化物电解质之间构筑物理屏障，抑制副反应	工艺相对成熟；有效降低界面阻抗；提升循环稳定性与倍率性能	涂层离子电导率不足；高电压稳定性有限；难以完全解决体积变化导致的机械接触失效	Ref. 27 Ref. 28
	Li₂SiO₃
	LiNbO₃
先进功能涂层	Li₂O-ZrO₂	不仅提供物理隔离，更注重涂层材料本身的高离子导、结构稳定或界面亲和性	更高的锂离子传输性能；更好的高电压稳定性；部分涂层(如Li₇TaO₆)可同时实现体相掺杂，协同改性	合成工艺更复杂，对厚度与均匀性控制要求高；成本可能较高	Ref. 29-34
	Li₇TaO₆
	Li₃PO₄
非氧化物/梯度涂层	DLC(类金刚石碳)	构建热力学更稳定的界面，或形成成分/性能渐变的梯度结构，以完美匹配两侧材料	化学/电化学稳定性，从根本上抑制副反应；梯度层能实现应力缓冲和离子传输的平滑过渡；部分涂层（如氟化物）具有优异的高压稳定性	制备工艺复杂，难以大规模应用(如原子层沉积)；非氧化物涂层的离子电导率需精细调控	Ref. 9 Ref. 35-36
	Li-Ta-O-F
	Li₃P_1+xO₄S_4x

图2 (a) 铟锂/钴酸锂电池的阻抗 (Z) 和充放电曲线[27]；(b) 无涂层、SiO2 涂层和 Li2SiO3 涂层钴酸锂全固态电池在第一次充电至 4.6V 后的阻抗曲线(vs. Li) [28]；(c) LCO内核上原位形成LCTO涂层的流程示意图以及改性后电池循环与倍率性能[29]。

Fig.2 (a) Impedance (Z) and charge-discharge curves of an In-Li/LCO battery[27]; (b) Impedance curves of uncoated, SiO2-coated, and Li2SiO3-coated LCO all-solid-state batteries after the first charge to 4.6V (vs. Li) [28]; (c) Schematic diagram of the in-situ formation process of an LCTO coating on the LCO core, and the cycling and rate performance of the modified battery[29].

图3 (a) L7TaO包覆NCM811合成示意图、PNCM811 和 L7TaO-1wt% 在 1C注:下的长循环曲线[34];(b) NMC811初级粒子(粉红色)与离子导电和梯度锂梯度Li3P1+xO4S4x涂层示意图及电池循环性能[9];(c) ASSB的倍率性能以及高压循环性能[35];(d) NCM811表面重建过程示意图以及高压循环性能[36]。

Fig.3 (a) Schematic diagram of the L7TaO-coated NCM811 synthesis process and long-term cycling curves of pristine NCM811 and L7TaO-1wt% at 1 C[34]; (b) Schematic diagram of an NMC811 primary particle (pink) with an ion-conductive gradient Li3P1+xO4S4x coating, and the corresponding battery cycling performance[9]; (c) Rate capability and high-voltage cycling performance of the ASSB[35]; (d) Schematic diagram of the surface reconstruction process of NCM811 and its high-voltage cycling performance[36].

表2 不同功能涂层作用机理及实现效果

Table 2 Mechanisms and Implementation Effects of Different Functional Coatings

核心功能	涂层材料	作用机理	实现效果	代表性文章
稳定界面 & 抑制副反应	Li₂ZrF₆(LZF)非晶/纳米晶涂层	热力学稳定以及抑制界面降解	保护层功能更持久，从根本上消除了界面相互作用的动力学障碍，实现超长循环寿命	Ref. 38
稳定界面 & 抑制副反应	离子-电子混合导电层(In-cPAN)	配位稳定；动态稳定界面	通过化学键合实现界面强化，并构建动态稳定的电极/电解质界面，显著抑制副反应	Ref. 41
提供快速锂离子传输路径	Li_1.175Nb_0.645Ti_0.4O₃(LNTO)涂层	原位形成离子导体	不仅降低了初始界面电阻，更在循环过程中构建稳定的高速离子通道，大幅提升倍率性能	Ref. 37
提供快速锂离子传输路径	铁电体(GClO₄)涂层	构建内建电场	通过电学机制而非传统的化学/物理机制，为界面离子传输提供全新驱动力，突破动力学瓶颈	Ref. 39
表面重构（变害为利）	Li₃VO₄ (LVO)涂层	原位转化	清除了表面残锂这一副反应“引发剂”；构建了能抑制副反应和结构滑移的稳定界面层	Ref. 36
表面重构（变害为利）	Li-Ta-O-F电解质涂层	原位转化	将有害物质转化为有益功能层，工艺简单，为高电压下稳定工作提供了关键界面保障	Ref. 35
多机制协同	LNTO涂层	协同：离子传输+界面稳定	通过多种元素的不同作用，协同实现了界面的全面稳定与动力学优化	Ref. 37
多机制协同	TNO包覆+Ti掺杂	协同：物理隔绝+体相锚定	实现了从“界面”到“体相”的协同增强，是应对高电压、高镍正极复杂挑战的典范策略	Ref. 40

图4 (a) 离子通过 LNO 和 LNTO 夹层的离子传输示意图[37]；(b) LZF-LCO 的结构SEM和EDS图谱[38]；(c) GClO4包覆结构及全固态电池的示意图[39]。

Fig.4 (a) Illustration of ion transport through LNO and LNTO interlayers at the interface[37]; (b) SEM and EDS Mapping of the LZF-LCO Structure [38]; (c) Schematic diagram of the GClO4 coating structure and the all-solid-state battery[39].

图5 (a) P-NCM 和LVO-NCM在循环过程中的结构演变示意图[36]；(b) SCNCM的界面失效机制示意图和 DC-TNO@SCNCM 的协同改性功能机制示意图[40]；(c) 多尺度Li||NCM811和Li||In-cPAN@NCM811固态电池模型示意图[41]。

Fig.5 (a) Schematic diagram of the structural evolution of P-NCM and LVO-NCM during cycling[36]; (b) Schematic diagram of the interfacial failure mechanism of SCNCM and the synergistic modification mechanism of DC-TNO@SCNCM[40]; (c) Schematic diagram of multi-scale models for Li||NCM811 and Li||In-cPAN@NCM811 all-solid-state batteries[41].

表3 电解质改性策略、机理及优缺点

Table 3 Electrolyte Modification Strategies， Mechanisms， and Advantages/Disadvantages

电解质改性策略	核心机理	优点	局限性	代表性文章
单元素掺杂	在电解质晶格内部中引入不同的单种元素，改变晶格体积和化学环境，构建富氟界面，增强空气/水稳定性等	工艺路线相对简单，易与现有球磨/固相合成放大；可以在保持较高离子电导率的前提下同时提高界面稳定性和空气稳定性；适合针对特定失效机理进行“定向设计”	掺杂量和占位(阳/阴离子位)存在较窄窗口；含Ag等贵/稀元素时成本和资源可持续性受到限制；掺杂多为体相调控，对高度不均匀的界面/颗粒接触问题缓解有限	Ref. 45–48
多元素掺杂	引入多种不同种元素进入电解质晶格，调整电解质晶格结构，协同提高电解质电导率、稳定性等	多种元素可分工协作，实现导电率、界面稳定性、空气稳定性和机械性能的多目标优化	双掺杂的掺杂量比例优化困难	Ref. 49–55
无机物表面包覆	在硫化物电解质颗粒表面沉积无机薄层，构建电子绝缘/离子导电的界面缓冲层	不改变电解质主体相结构，对体相σ影响小；可在成膜之后整体包覆，兼容多种硫化物体系；适配高压	工艺复杂度和成本较高；涂层厚度与均匀性窗口窄；部分氧化物/氟化物涂层本身与硫化物存在热力学反应风险	Ref. 56 Ref. 58
有机物表面包覆	利用有机分子在电解质表面形成致密吸附层，外侧提供疏水有机链段，内侧与硫化物牢固结合；同时可在分子结构中引入含Li⁺亲和基团，保证界面附近的离子传导能力	可显著改善硫化物在潮湿空气中的稳定性；有机层柔性好，能够缓冲压实及循环过程中的应力集中；制备工艺适合复杂形状与大面积电解质膜	需要选择与硫化物化学惰性的溶剂和前驱体；有机层本身的电化学窗口相对有限，在高电压/高温下可能分解；若亲离子基团设计不当，会明显降低界面Li⁺传导	Ref. 57
聚合物共混	构建“硫化物刚性骨架+聚合物柔性网络”的双连续结构：硫化物提供高速Li⁺传导主通道，聚合物填充孔隙、提高膜的柔性和韧性，减小界面接触电阻	兼具较高σ(10^-3–10^-4 S·cm^-1)与优异机械顺应性，易实现自由支撑薄膜，适配卷绕/叠片工艺	制备工艺中所使用溶剂等应与硫化物电解质相适宜；聚合物需要对正负极及电解质稳定，以获得稳定界面	Ref. 59-60

表3 电解质改性策略、机理及优缺点

Table 3 Electrolyte Modification Strategies， Mechanisms， and Advantages/Disadvantages

电解质改性策略	核心机理	优点	局限性	代表性文章
单元素掺杂	在电解质晶格内部中引入不同的单种元素，改变晶格体积和化学环境，构建富氟界面，增强空气/水稳定性等	工艺路线相对简单，易与现有球磨/固相合成放大；可以在保持较高离子电导率的前提下同时提高界面稳定性和空气稳定性；适合针对特定失效机理进行“定向设计”	掺杂量和占位(阳/阴离子位)存在较窄窗口；含Ag等贵/稀元素时成本和资源可持续性受到限制；掺杂多为体相调控，对高度不均匀的界面/颗粒接触问题缓解有限	Ref. 45–48
多元素掺杂	引入多种不同种元素进入电解质晶格，调整电解质晶格结构，协同提高电解质电导率、稳定性等	多种元素可分工协作，实现导电率、界面稳定性、空气稳定性和机械性能的多目标优化	双掺杂的掺杂量比例优化困难	Ref. 49–55
无机物表面包覆	在硫化物电解质颗粒表面沉积无机薄层，构建电子绝缘/离子导电的界面缓冲层	不改变电解质主体相结构，对体相σ影响小；可在成膜之后整体包覆，兼容多种硫化物体系；适配高压	工艺复杂度和成本较高；涂层厚度与均匀性窗口窄；部分氧化物/氟化物涂层本身与硫化物存在热力学反应风险	Ref. 56 Ref. 58
有机物表面包覆	利用有机分子在电解质表面形成致密吸附层，外侧提供疏水有机链段，内侧与硫化物牢固结合；同时可在分子结构中引入含Li⁺亲和基团，保证界面附近的离子传导能力	可显著改善硫化物在潮湿空气中的稳定性；有机层柔性好，能够缓冲压实及循环过程中的应力集中；制备工艺适合复杂形状与大面积电解质膜	需要选择与硫化物化学惰性的溶剂和前驱体；有机层本身的电化学窗口相对有限，在高电压/高温下可能分解；若亲离子基团设计不当，会明显降低界面Li⁺传导	Ref. 57
聚合物共混	构建“硫化物刚性骨架+聚合物柔性网络”的双连续结构：硫化物提供高速Li⁺传导主通道，聚合物填充孔隙、提高膜的柔性和韧性，减小界面接触电阻	兼具较高σ(10^-3–10^-4 S·cm^-1)与优异机械顺应性，易实现自由支撑薄膜，适配卷绕/叠片工艺	制备工艺中所使用溶剂等应与硫化物电解质相适宜；聚合物需要对正负极及电解质稳定，以获得稳定界面	Ref. 59-60

图6 (a) LiF替代LiCl改性LSPCl的机理示意图[45]以及(b)阻抗图[46]；(c) Ag掺杂的LPSCl示意图[48]；(d) Li2AlO2改性硫化物电解质的机理与性能图[49]；(e) Ge、Cl双掺杂的LGPS提升离子跃迁能力[50]；(f) Li5.8P0.9Cu0.1S4.5Cl1.3Br0.2全固态电池性能[51]；(g) Li-In/ Li5.55Si0.05P0.95S4.4Cl0.75Br0.75O0.1/NCM811@LNO全电池性能[52]。

Fig.6 (a) Schematic diagram of the mechanism for modifying LSPCl with LiF as a substitute for LiCl[45]and (b) the corresponding impedance plot[46]; (c) Schematic diagram of Ag-doped LPSCl[48]; (d) Mechanism and performance plots of Li2AlO2-modified sulfide electrolyte[49]; (e) Enhanced ion migration capability achieved by co-doping LGPS with Ge and Cl[50]; (f) Performance of the Li5.8P0.9Cu0.1S4.5Cl1.3Br0.2 all-solid-state battery[51]; (g) Performance of the Li-In/ Li5.55Si0.05P0.95S4.4Cl0.75Br0.75O0.1/NCM811@LNO full cell[52].

图7 (a) LSO保护层作用机制图[56]；(b) UDSH@LPSC复合电解质制备工艺图[57]；(c) HCPE电解质体系全固态电池性能[59]；(d) 改性LPSCl-PEO与未改性LPSCl电解质全固态电池性能对比[60]。

Fig.7 (a) Mechanism diagram of the protective layer of LSO[56]; (b) Preparation process diagram of the UDSH@LPSC composite electrolyte[57]; (c) Performance of the all-solid-state battery using the HCPE electrolyte system[59]; (d) Performance comparison of all-solid-state batteries using modified LPSCl-PEO versus unmodified LPSCl electrolyte[60].

图8 (a) LiPO2F2在正极侧的作用机制及全固态电池性能[65]；(b) 掺杂LiPO2F2提升电极的致密性[66]；(c) LiDFOB掺杂改性正极的作用机制以及全固态电池性能[67]。

Fig.8 (a) Mechanism of LiPO2F2 at the cathode interface and the corresponding all-solid-state battery performance[65]; (b) Enhanced electrode compactness through LiPO2F2 doping[66]; (c) Modification mechanism of LiDFOB doping on the cathode and the performance of the all-solid-state battery[67].

图9 (a) 导电粘结剂PPC-ICP提升电极离子传输示意图及全固态电池性能[71]；(b) 共溶NBR和LiTFSI粘结剂提升电极离子传输示意图及全固态电池性能[72]；(c) 粘结剂提升电极离子传输及致密性[73]。

Fig.9 (a) Schematic diagram of the conductive binder PPC-ICP enhancing ion transport in the electrode and the corresponding all-solid-state battery performance[71]; (b) Schematic diagram of the co-dissolved NBR and LiTFSI binder improving electrode ion transport and the corresponding all-solid-state battery performance[72]; (c) Enhancement of electrode ion transport and compactness by the binder[73].

表4 结构工程改性机理及实现效果

Table 4 Modification Mechanisms and Implementation Effects of Structural Engineering

结构工程方向	针对问题	核心机理	实现效果	代表性文章
活性材料粒径调控	厚电极下活性物质未充分活化、CAM-SE接触失效	将CAM粒径与SE粒径匹配，在高体积分数CAM条件下形成离子连续相，减小电子输运距离，实现离子/电子双渗流	通过调控NCM和LPS颗粒尺寸并改变CAM含量，在70%CAM含量下实现150 mAh/g初始放电比容量	Ref. 77-78
活性材料形貌工程	循环过程中产生应力集中，二次颗粒易开裂	通过采用小尺寸单晶或定向柱状一次颗粒，缩短Li⁺扩散路径，减少晶界阻力和应力集中	通过使用小尺寸单晶 NCM811，在35.67 mg/cm² 的高质量负载下，在 2.72–4.4 V 电压范围内循环500次后稳定性为100%	Ref. 63 Ref. 79-80
固态电解质粒径/级配	离子通道中断、离子迂曲度高，厚电极极化严重	使用更小粒径甚至分级SE填充CAM颗粒间的孔隙，降低离子路径的迂曲度 τ_SE，提升有效离子电导σ_i^eff	通过双步研磨工艺控制电解质粒径，在0.6 C的倍率下，初始放电容量可达179 mAh/g，过电势60 mV	Ref. 16 Ref. 81-83
导电剂与导电网络设计	低碳含量下复合正极内部电子网络不连续	通过控制结晶度、采用合适导电剂碳材料搭建长程电子通路，实现电子渗流	室温下，使用rGO的全固态电池循环100圈容量保持率为97%，库仑效率为99.8%，电池在60 °C，1 C下循环1000圈容量保持率≈100%	Ref. 87-89
导电剂界面层设计	传统碳材料触发严重的电解质界面副反应，导致阻抗上升	在导电剂表面引入导电聚合物，提供电子通路，阻隔碳与电解质的直接接触，抑制副反应	将PEDOT半导体界面层引入导电剂表面，在1 C下仍可输出超过100 mAh/g(较未改性提升约10倍)	Ref. 90
组分配比/结构设计	高CAM体积分数、厚电极下离子/电子通路失衡，	通过传输线模型、电阻网络、梯度设计等方法寻找使 σᵢᵉᶠᶠ 与 σₑᵉᶠᶠ 相当的CAM/SE/碳体积分数窗口，避免单一通道成为瓶颈	通过纵向梯度分层设计的电池在3.22 mA/cm²下放电比容量为49±10 mAh/g，显著优于等组分电极	Ref. 91-96
堆压–微结构协同与力学稳定性设计	堆叠压力与实际工况矛盾	通过多物理场建模以及实验验证，研究复合正极中堆压对微结构、接触面积、反应分布的影响，提出“临界堆压”窗口	在理论“临界堆压”17 MPa下，单晶NMC532在0.1 C下初始放电容量为146.94 mAh/g，接近理论容量	Ref.97

表4 结构工程改性机理及实现效果

Table 4 Modification Mechanisms and Implementation Effects of Structural Engineering

结构工程方向	针对问题	核心机理	实现效果	代表性文章
活性材料粒径调控	厚电极下活性物质未充分活化、CAM-SE接触失效	将CAM粒径与SE粒径匹配，在高体积分数CAM条件下形成离子连续相，减小电子输运距离，实现离子/电子双渗流	通过调控NCM和LPS颗粒尺寸并改变CAM含量，在70%CAM含量下实现150 mAh/g初始放电比容量	Ref. 77-78
活性材料形貌工程	循环过程中产生应力集中，二次颗粒易开裂	通过采用小尺寸单晶或定向柱状一次颗粒，缩短Li⁺扩散路径，减少晶界阻力和应力集中	通过使用小尺寸单晶 NCM811，在35.67 mg/cm² 的高质量负载下，在 2.72–4.4 V 电压范围内循环500次后稳定性为100%	Ref. 63 Ref. 79-80
固态电解质粒径/级配	离子通道中断、离子迂曲度高，厚电极极化严重	使用更小粒径甚至分级SE填充CAM颗粒间的孔隙，降低离子路径的迂曲度 τ_SE，提升有效离子电导σ_i^eff	通过双步研磨工艺控制电解质粒径，在0.6 C的倍率下，初始放电容量可达179 mAh/g，过电势60 mV	Ref. 16 Ref. 81-83
导电剂与导电网络设计	低碳含量下复合正极内部电子网络不连续	通过控制结晶度、采用合适导电剂碳材料搭建长程电子通路，实现电子渗流	室温下，使用rGO的全固态电池循环100圈容量保持率为97%，库仑效率为99.8%，电池在60 °C，1 C下循环1000圈容量保持率≈100%	Ref. 87-89
导电剂界面层设计	传统碳材料触发严重的电解质界面副反应，导致阻抗上升	在导电剂表面引入导电聚合物，提供电子通路，阻隔碳与电解质的直接接触，抑制副反应	将PEDOT半导体界面层引入导电剂表面，在1 C下仍可输出超过100 mAh/g(较未改性提升约10倍)	Ref. 90
组分配比/结构设计	高CAM体积分数、厚电极下离子/电子通路失衡，	通过传输线模型、电阻网络、梯度设计等方法寻找使 σᵢᵉᶠᶠ 与 σₑᵉᶠᶠ 相当的CAM/SE/碳体积分数窗口，避免单一通道成为瓶颈	通过纵向梯度分层设计的电池在3.22 mA/cm²下放电比容量为49±10 mAh/g，显著优于等组分电极	Ref. 91-96
堆压–微结构协同与力学稳定性设计	堆叠压力与实际工况矛盾	通过多物理场建模以及实验验证，研究复合正极中堆压对微结构、接触面积、反应分布的影响，提出“临界堆压”窗口	在理论“临界堆压”17 MPa下，单晶NMC532在0.1 C下初始放电容量为146.94 mAh/g，接近理论容量	Ref.97

图10 (a) 不同粒径NCM622的全固态电池性能[77]；(b) 不同FeS2粒径对全固态电池性能的影响[78]；(c) 单晶和多晶NCM532体系全固态电池性能[79]；(d) S-NCA和SM-NCA在100圈循环后的SEM图[63]。

Fig.10 (a) Performance of all-solid-state batteries using NCM622 with different particle sizes[77]; (b) Effect of FeS2 particle size on the performance of all-solid-state batteries[78]; (c) Performance comparison of all-solid-state batteries based on single-crystal and polycrystalline NCM532 systems[79]; (d) SEM images of S-NCA and SM-NCA after 100 cycles[63].

图11 (a) 5 μm NCM匹配不同粒径电解质的性能[16]；(b) dAM/dSE粒径匹配影响参数[81]；(c) dCAM/dSE与电池放电容量、电导率关系图[82]；(d) 高能球磨参数对电极致密度的影响[83]。

Fig.11 (a) Performance of 5μm NCM paired with solid-state electrolytes of different particle sizes[16]; (b) Parameters showing the influence of dAM/dSE particle size matching[81]; (c) Relationship between dCAM/dSE and battery discharge capacity/conductivity[82]; (d) Effect of high-energy ball milling parameters on electrode density[83].

图12 (a) 不同导电剂混合电极结构示意图[86]；(b) 不同导电剂电极内部示意图及全固态电池性能对比[87]；(c) 电子/离子传输连续性示意图及退化分析图[89]；(d) 半导体PEDOT界面层降低界面阻抗示意图[90]。

Fig.12 (a) Schematic diagram of composite electrode structures with different conductive agents[86]; (b) Internal schematic of electrodes with different conductive agents and corresponding all-solid-state battery performance comparison[87]; (c) Schematic of electron/ion transport continuity and corresponding degradation analysis[89]; (d) Schematic illustrating the reduction of interfacial resistance by a semiconducting PEDOT interlayer[90].

图13 (a) 阻抗-传输线模型[91]；(b) 电阻网络模型[93]。

Fig.13 (a) Impedance-transmission line model[91]; (b) Resistance network model[93].

图14 (a) 混合电极内部各组分分布图[95]；(b) 三层梯度示意图及组分含量与性能关系[96]；(c) 临界堆压对电池内部影响示意图[97]；(d) 隔膜厚度-正极架构的协同路线示意图[98]。

Fig.14 (a) Distribution of components within the composite electrode[95]; (b) Schematic of the three-layer gradient structure and the relationship between component content and performance[96]; (c) Schematic illustrating the effect of critical stack pressure on the battery interior[97]; (d) Schematic of the synergistic approach between separator thickness and cathode architecture[98].

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