Tailored CEI architectures to boost high-performance solid-state Zn-ion batteries

Yitao Zhao abc, Lingbiao Meng a, Linhong Mao ef, Yan Nie a, Siyao Jiang a, Guosen Zhou a and Jingjing Yuan *d
aJiangsu Province Engineering Research Center of Special Functional Textile Materials, Changzhou Vocational Institute of Textile and Garment, Changzhou, Jiangsu 213164, China
bJiangsu Key Laboratory of Materials and Technologies for Energy Storage, College of Material Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing, Jiangsu 211106, China
cJiangsu Baoyuan High Tech Electrician Co., Ltd, Yangzhou, Jiangsu 225800, China
dChangzhou University, Changzhou, Jiangsu 213164, China. E-mail: happyyjj1988@163.com
eHarbin Aircraft Industry Group Co., Ltd, Harbin, 150066, China
fKey Laboratory of Superlight Materials and Surface Technology, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China

Received 12th September 2025 , Accepted 20th October 2025

First published on 21st October 2025


Abstract

Solid-state zinc-ion batteries (ZIBs) have emerged as a pivotal candidate for next-generation energy storage systems due to their inherent safety and environmental compatibility. However, critical challenges at the cathode–electrolyte interface (CEI), including sluggish ion transport kinetics, mechanical instability, and parasitic side reactions, persistently hinder their performance breakthroughs. To tackle these limitations, this review presents a categorized overview of CEI modification strategies based on interfacial engineering, which aim to systematically modulate electrode–electrolyte interactions. These strategies include dynamic adaptive regulation via in situ reconstruction, defect engineering for activating inert sites, heterojunction band engineering to optimize charge transfer pathways, and biomimetic dynamic bonding mechanisms that boost interfacial stability through self-healing capabilities. Additionally, solid electrolyte modifications significantly improve interfacial durability and synergistic strategies further reinforce interfacial chemical and mechanical robustness. This review consolidates recent advancements in these interfacial optimization mechanisms and critically discusses future research directions, including multiscale characterization techniques, intelligent material design paradigms, and scalable manufacturing technologies. These insights provide a theoretical framework and technical roadmap for developing high-stability, intelligent energy storage interfaces, paving the path for the practical deployment of advanced solid-state ZIBs.


1. Introduction

Zinc-ion batteries (ZIBs) have shown promising application prospects in the new generation of energy storage systems due to their abundant resources, low cost, high safety, and high theoretical capacity.1–4 However, traditional liquid ZIBs are severely limited by the inherent defects of the electrolyte,5–7 such as uncontrollable growth of zinc dendrites, hydrogen evolution reactions (HER), and electrolyte leakage, which significantly restrict the improvement of their cycle life and energy density.8–10 Exploring novel solid-state ZIBs has become a key path to break through the technical bottlenecks of current liquid ZIBs.11–13

Solid-state zinc-ion batteries (SSZIBs) can effectively suppress the growth of zinc dendrites and extend the battery's cycle life due to the presence of solid-state electrolytes.14–16 Moreover, the robust tolerance to high temperatures and the inherently non-toxic nature of solid-state electrolytes further underscore their enhanced safety characteristics and ecological benignity.17–21 Furthermore, advancements in the synthesis of novel solid-state electrolytes, possessing exceptional ionic conductivity and paired with high-capacity cathode materials, have led to a substantial increase in the energy density of SSZIBs, progressively narrowing the gap with lithium-ion batteries.22–26

SSZIBs have become ideal candidates for grid scale energy storage systems and distributed energy, while also demonstrating significant advantages in professional applications including low altitude aircraft and flexible wearable devices.27–30 Nevertheless, the development of SSZIBs faces several challenges, including volume expansion, HER, and surface passivation of the zinc anode during the deposition/striping process, which remain key issues to be addressed.31–34 To solve these problems, the scientific community has actively explored various modification strategies for solid-state electrolytes, such as the use of 2D layered natural solid-state electrolyte materials,35 sol–gel transition hydrogel electrolytes,36 and deep eutectic electrolytes.37

Although significant progress has been made in anode modification research, compared to the extensive studies on the anode, cathode modification work still lags behind, especially the interface between the cathode and the solid-state electrolyte (CEI), which has not received sufficient attention for a long time.38–40 This interface plays a crucial role in the ion transport kinetics, mechanical stability, and long-term cycling performance of the cathode. Insufficient interface compatibility not only causes charge transfer resistance to increase sharply, but also results in stress accumulation, which in turn brings about interface contact failure.41–43 In severe cases, it may even lead to the collapse of the cathode material structure, ultimately causing a rapid decline in battery capacity.44–46 Therefore, optimizing the CEI interface is a crucial task to comprehensively enhance the performance of SSZIBs. Currently, researchers are actively exploring a series of optimization techniques, mainly focusing on the interface modification of cathode materials, modification strategies for solid-state electrolytes, and other CEI engineering designs, aiming to enhance the CEI interface and improve the overall performance of SSZIBs, as shown in Fig. 1.47–49 These techniques not only represent the cutting-edge progress in CEI interface optimization, but also provide innovative ideas for solving key issues, such as ion conduction, electronic insulation, and structural stability at the interface in SSZIBs.


image file: d5ta07455j-f1.tif
Fig. 1 Current optimization strategy for CEI interface in SSZIBs.

2. Interface modification of cathode materials

To alleviate the problems of interface structure evolution, low ion transport efficiency, and interfacial side reactions faced by cathode materials in ZIBs during cycling, researchers are exploring multiple strategies, including dynamic adaptive interface engineering, construction of heterostructures, biomimetic self-healing interface layers, and multi-field coupled interface design as seen from Fig. 2.49–53
image file: d5ta07455j-f2.tif
Fig. 2 Schematic illustration of interface modification strategies for cathode materials.

2.1 Dynamic adaptive interface engineering

Traditional cathode interface modification strategies, such as pre-doping, often fail to adapt to the dynamic structural changes during battery cycling, resulting in performance degradation.54–56 Importantly, these challenges are further amplified in solid-state systems due to the inherently poor interfacial contact between the cathode and solid-state electrolyte. In recent years, in situ electrochemical reconstruction technology has emerged as a key breakthrough to address this challenge, as it not only adapts to cathode structural changes but also synchronously optimizes the interface of cathode and solid-state electrolyte. Notably, this technology exhibits differential application adaptability across various cathode materials. For V-based and Mn-based oxides, it can easily achieve active site activation and interface optimization through lattice reconstruction, whereas for phosphate-based cathodes, it is necessary to regulate the electrochemical window to match the intrinsic stability of them, avoiding structural collapse during the reconstruction process. For instance, Zhang et al. activated the non-electrochemically active ZnV2O4 spinel cathode through an in situ electrochemical amorphization mechanism to unlock ultrafast reaction kinetics electrodes. It was found that the long-range ordered ZnV2O4 crystals could be reconstructed into short-range ordered Zn0.44V2O4 quantum dots, showing significantly increased active sites, shortened diffusion paths, and enhanced the capture ability of Zn2+. This reconstructed amorphous electrode maintained excellent storage capacity (251 mA h g−1) even at low temperatures (−25 °C), and Warburg impedance was significantly reduced that defined as the impedance response under diffusion control. This in situ electrochemical amorphization mechanism is expected to be applied to high-power and low-temperature SSZIBs.57

In addition to the in situ electrochemical reconstruction technology, oxygen vacancies have a significant impact on interfacial reaction kinetics through their dynamic evolution. Dong et al. have successfully prepared oxygen-deficient amorphous MnO2 ultrathin nanosheets by introducing sodium carboxymethyl cellulose (CMC) as a capping agent, achieving dual regulation of material structure and electronic coordination, as shown in Fig. 3.58 Moreover, the concentration and distribution of oxygen vacancies can be precisely controlled through external field, such as light, electricity and heat. Ultraviolet light irradiation can induce high-density oxygen vacancies on the surface of MnO2, reducing the adsorption energy of Zn2+ and increasing the diffusion coefficient.59 Additionally, thermal activation and recombination promote the aggregation of oxygen vacancies to form ordered nanodomains, establishing rapid ion diffusion channels and improving rate performance.


image file: d5ta07455j-f3.tif
Fig. 3 Energy storage mechanism diagram of CMC–MnO2 (a), reproduced from ref. 58, with permission from Adv. Funct. Mater., copyright 2024. MD simulation snapshots for Zn2+ diffusion in the bulk electrode and amorphous electrode at 3 M Zn(OTf)2 in water (b) and (c). Schematic illustration of the ultrafast ion storage mechanism for the amorphous electrode (d), reproduced from ref. 57, with permission from Adv. Funct. Mater., copyright 2023.

2.2 Construction of heterostructures

The interfaces of traditional composite materials are often randomly mixed, which can lead to uneven charge distribution and stress concentration.60–63 It has been found that heterostructured materials formed by combining with 2D high-conductivity materials (such as graphene, MXene) can accelerate ion diffusion kinetics and reduce ion diffusion barriers due to the introduction of built-in electric fields around the heterointerfaces, thereby facilitating the storage of more Zn2+.64,65 At the same time, strong interactions such as chemical bonds and the van der Waals forces can stabilize charge distribution, improve structural stability, and extend cycle life.66–68 For example, Huang et al. prepared a 2D heterostructured HVO@Ti3C2 that rich in V–O–Ti hetero-bonds through self-assembly electrostatic adsorption as shown in Fig. 4. The heterostructured material delivered an ultra-high capacity of 457.1 mA h g−1 at 0.2 A g−1, a value significantly higher than the theoretical capacity of pure HVO. HVO@Ti3C2 maintained excellent cycle stability with 88.9% capacity retention after 1000 cycles. This heterostructured material exhibited dynamic reversible interfacial coupling during charging and discharging, which activated the faradaic activity of MXene that originally had no capacity contribution in ZIBs, making it an additional electron acceptor/donor and providing additional capacity contribution.69
image file: d5ta07455j-f4.tif
Fig. 4 The change of interface structure when 0, 1, 2, 3, and 4 Zn2+ are inserted in the heterointerface (a), the PDOS of V, O, and Ti after inserting 0 and 4 Zn2+, respectively (b), reproduced with ref. 69 with permission from Adv. Funct. Mater., copyright 2023.

Furthermore, the band bending and carrier transport characteristics at the heterojunction interface have a decisive influence on electrochemical performance.70–74 Through the regulation of Schottky barriers, passivation of interface states, and modulation of the space charge region, the efficiency of charge transport can be substantially improved. For instance, Bin et al. designed a porous Mott–Schottky heterojunction of a composed phase of Fe0.12V2O5 and Fe2V4O13 as shown in Fig. 5, whose built-in electric field characteristics can maximize the interface effect, promote charge transfer in the bulk electrode, and thereby achieve excellent electrochemical performance for Zn2+ storage.75


image file: d5ta07455j-f5.tif
Fig. 5 Preparation process of HVO@Ti3C2 2D heterostructure material. The preparation of HVO@Ti3C2 includes three main steps: etching and exfoliation of Ti3C2 MXene, in situ liquid-phase growth exfoliation of V5O12, and electrostatic adsorption for self-assembly (a), reproduced from ref. 69, with permission from Adv. Funct. Mater., copyright 2023. The ex situ XRD patterns (b) and (c); SEM and TEM images of the (e) and (f) FeVO-1. HRTEM images and STEM-EDS elemental mappings of (g) and (h) FeVO-1, reproduced from ref. 75, with permission from Nano Lett., copyright 2025.

2.3 Biomimetic self-healing interface layer

By drawing inspiration from the self-repair mechanisms of biological tissues and incorporating dynamic covalent and non-covalent bonds, an intelligent interface layer is designed to dramatically boost the cycling stability of electrodes. The polymer network containing hydrogen bonds can undergo bond reorganization under cyclic stress, achieving efficient healing of microcracks.77–81 Notably, an interface based on multiple hydrogen bonds can dynamically adapt in aqueous environments to mend deep cracks and restore initial mechanical strength. For example, Li et al. modified the hydrophilic α-MnO2 surface with a conductive polymer film of polydopamine (PDA) with appropriate hydrophobicity through in situ polymerization, constructing a biomimetic cathode–electrolyte interface with a cell membrane-like structure as shown in Fig. 6, thereby achieving selective and efficient transport of Zn2+.82 Additionally, inspired by the wet adhesion of mussels to various substrates through the secretion of dopamine, Li et al. modified the surface of MnO2 nanorods with a polydopamine (PDA) film, constructing a PDA-coated MnO2 composite electrode, which promoted the desolvation process of hydrated Zn2+ and thereby improved the electrochemical performance of ZIBs as shown in Fig. 7.83
image file: d5ta07455j-f6.tif
Fig. 6 ESP mapping of [Zn(H2O)6]2+, DA, and DA–Zn2+ clusters (a), Adsorption energy of H2O molecule on the MnO2 and DA substrate. Inset is the corresponding absorbed model (b), schematic of the insertion mechanism of H+ and Zn2+ in the PDMO cathode (c), reproduced with ref. 76 with permission from J. Mater. Chem. A, copyright 2025.

image file: d5ta07455j-f7.tif
Fig. 7 The simulation diagram of the H+ and Zn2+ insertion mechanism on the PMC-8 cathode (a), the design principle for the amphiphilicity of plasma membrane and hydrophobic conductive PEDOT film (b), schematic diagram of hydrated zinc ion desolvation behavior on the PEDOT film (c), reproduced from ref. 82, with permission from Angew. Chem., Int. Ed., copyright 2023. Schematic diagram of bio-inspired anionic polyelectrolyte from seaweed absorbing metal cations from the seawater (d), schematic diagrams of the bare Zn and the polyanionic electrolyte coated Zn plating behaviours, where polyanionic layer coating induces a well-aligned Zn2+ accelerating channel, while bare Zn possesses a fluffy deposition (e), reproduced from ref. 81, with permission from Small, copyright 2022.

2.4 Multi-field coupled interface design

Intervening in the material growth process with physical external fields can achieve the directional optimization of interface properties. By adjusting the electric field, including enhancing and unifying the electric field strength, and coupling the external magnetic field/pressure field/thermal field with the electric field, the uniform and rapid diffusion of Zn2+ can be promoted.84–87 For instance, Na et al. leveraged the piezomagnetic effect to equip the conventional artificial protective layer with targeted regulation capabilities for Zn2+ migration and deposition behaviors. This resulted in a magnetic field-induced phase transformation, creating an interlaced tunnel structure that effectively shortened the ion diffusion path.88,89 Based on this, the study of interface reaction mechanisms under multi-field coupling has become an important research direction for the future, including the development of thermally stable interface layers to suppress thermal runaway in electrothermal coupling, the design of piezoelectric compensation layers to balance charge distribution in force-electric coupling, and the construction of Z-type heterojunctions to promote carrier separation and avoid interface corrosion in coupling.

3. Modification strategies for solid-state electrolytes

Solid-state electrolytes have evolved breakthrough technological paths focusing on interface engineering innovation and hydrogen bond modified electrolyte as shown in Fig. 8.90–92 Specifically, the interface resistance is effectively reduced and the ion transmission efficiency is improved by accurately controlling the interaction between the electrolyte and the electrode.93–95 Novel solid-state electrolyte materials, such as novel polymers and inorganic ceramics, are being explored to enhance the ionic conductivity and mechanical strength of electrolytes.96–99 In addition, modifying the internal structure of solid electrolytes can enhance their mechanical properties and broaden their temperature range of use.100–102
image file: d5ta07455j-f8.tif
Fig. 8 Schematic illustration of modification strategies for solid-state electrolytes.

3.1 Interface engineering innovation

Traditional solid electrolyte interface modification mainly focuses on physical barriers to suppress side reactions on the cathode materials, such as metal dissolution and structural phase transition, while the latest strategies have developed into molecular design based regulatory systems.103–105 By accurately designing the functional group coordination network in solid electrolytes, researchers have successfully achieved intelligent regulation of Zn2+ solvation structure. For example, the abundant amino groups on the chitosan molecular chain impart a positively charged framework of the chitosan-based solid electrolyte, and the coordination effect of chitosan molecules with Zn2+ effectively modulates the homogenized electric field and ion concentration. In the field of interface chemical regulation, the innovative double layer barrier design breaks through the limitations of single protection. For example, Zhou et al. constructed a cobalt ferrite oxide magnetic functional layer on Zn foil, which controls Zn2+ migration via piezomagnetic effect to suppress dendrites, as shown in Fig. 9.106 In addition, the organic/inorganic biphasic solid electrolyte interface has been further designed, such as adding tris(2-cyanoethyl)phosphine (TCEP) to the electrolyte. The existence of TCEP promotes the decomposition of triflate (OTF) and generates inorganic components rich in ZnF2. This inner layer is rich in organic components and the outer layer is rich in inorganic components, which causes the transmission of Zn2+ to be regulated to a certain extent, which is manifested as a higher ion transport activation energy (34.58 kJ mol−1, compared to 24.61 kJ mol−1 in traditional electrolytes).107 The integration of gradient interface engineering with molecular dynamics simulation is catalyzing the transition from macroscopic modifications to atomic-level precision regulation.
image file: d5ta07455j-f9.tif
Fig. 9 Schematic illustration of the Zn nucleation and growth mechanisms of the (a) bare Zn and (b) CFO–Zn, reproduced with ref. 88 with permission from Energy Environ. Sci., copyright 2025. Schematic illustration of deposition mechanism in BE and ZS-CMIM0.1 electrolyte (c); schematic descriptions of EDL structure before and after introducing CMIM (d), reproduced with ref. 89 with permission from Angew. Chem., Int. Ed., copyright 2024.

3.2 Hydrogen bond modified electrolyte

The development of novel hydrogel materials has transcended conventional limitations of single-performance optimization, progressing towards the synthesis of multifunctional integrations. Hydrogel (Ur-SA) based on flexible urea (Ur) modified sodium alginate (SA) composite is used as a sensor device for the hydrogel electrolyte of SSZIBs. This biocompatible amido group and carboxyl group in Ur-SA gel can regulate the solvation structure of Zn2+, as well as the electrolyte/electrode interface generated in situ, the flexible Ur-SA-based screen-printed micro SSZIBs can provide stable and long-lasting energy supply to wearable sensing systems, and its capacity retention rate reaches 69.37% after 200 cycles at 1.2 A g−1.108 Notably, the hydrogen bond interaction mechanism exhibits good universality across different hydrogel electrolyte systems. For sodium alginate-based hydrogels, hydrogen bonds between amido/carboxyl groups and water molecules optimize Zn2+ solvation. For chitosan-based hydrogels, amino and hydroxyl groups form hydrogen bonds to enhance electrolyte retention and structural stability. For PVA-based systems, hydrogen bond regulation plays a core role in performance optimization. In the process of exploring the optimization of hydrogel electrolyte performance, the hydrogen bond regulation mechanism between different systems is universal. From the perspective of hydrogen bond microenvironment reconstruction, Li et al. proposed a delicate molecular bridging strategy to enhance compatibility between PVA and ZnSO4. By adding Ur, the broken intermolecular hydrogen bonds between PVA and H2O can be re-bound, thereby greatly improving the bearing capacity of ZnSO4 and inhibiting the salting effect as shown in Fig. 10.109
image file: d5ta07455j-f10.tif
Fig. 10 ESP mapping results of H2O and DMF (a), energy levels of H2O and DMF (b), the evolution of Zn anodes in PZ and PZD hydrogel electrolytes (c), reproduced with ref. 110 with permission from Small, copyright 2024. Schematic illustration about the fundamental mechanism of enhanced electrochemical performance by using the Gel-PUZ (d), reproduced with ref. 109 with permission from Angew. Chem., Int. Ed., copyright 2024.

The dynamic self-healing technology based on hydrogen bonding has achieved in situ repair of electrolytes with novel complex structures, providing a disruptive solution for flexible electronic devices. For instance, Shu et al. used the strong complexation between Zn2+ and chitosan and strong internal hydrogen bonding to propose an immersion-free self-healing hydrogel electrolyte for advanced wearable ZIBs. The hydrogel composed of Zn2+, chitosan and polyacrylamide achieved a long cycle life of 2000 times at 3 A g−1, with a capacity retention rate of 94.6%. When assembled into a Zn‖polyaniline bag battery, it maintains a stable energy output in harsh environments, such as pressure, folding, extrusion, twisting, penetration, and hammering, all showing good stability performance.110

In addition, the functionalized solid-state gel electrolyte also endows the SSZIBs with self-powering performance, which is attributed to the piezoelectric response property of the solid-state gel electrolyte.111,112 For example, Liu et al. constructed a gelatin sensor composed of stainless steel mesh coated with the active substance VO2, a polydimethylsiloxane isolation layer, a gelatin–chitosan composite film and zinc sheet electrode. The gelatin battery pressure sensor provides excellent pressure sensing performance in both static and dynamic modes as shown in Fig. 11.113 These breakthrough progress is driving the evolution of ZIBs to smart energy systems, showing unique advantages in wearable electronics, medical implantation and other fields.


image file: d5ta07455j-f11.tif
Fig. 11 Electrostatic potential mapping of DTPA–Na and H2O (a) and (b), 3D snapshots of (c) ZSO and (d) ZSO–DTPA obtained from MD simulations and partially enlarged snapshots of the solvation structure of Zn2+ (e) and (f), HOMO/LUMO energy levels of DTPA and H2O molecules (g), reproduced with ref. 113, with permission from Angew. Chem., Int. Ed., copyright 2024. The charge density difference when VO2+ (h), VO2+ (i), and Zn2+ (j) transfer in the ZnOTf-LDH individually, reproduced with ref. 114, with permission from Adv. Mater., copyright 2024.

4. Other CEI engineering designs

4.1 Synergistic strategies for building CEI and solid electrolyte interface (SEI)

The anode and cathode interface can be optimized simultaneously by introducing electrolyte additives. For example, Kang et al. added a novel electrolyte additive of diethylenetriamine pentaacetate sodium salt (DTPA–Na), so that a stable mesophase in multi-layered solid-state electrolyte is formed on the zinc anode and a stable cathode electrolyte mesophase is formed on the MnOOH cathode. This engineering method that synergizes the two mesophases effectively inhibits interfacial reactions, promotes uniform zinc deposition, and inhibits the growth of zinc dendrites, resulting in special cycle stability and self-discharge inhibition.114 The asymmetric battery using DTPA–Na achieved 32[thin space (1/6-em)]000 cycles at a high charging rate of 50 mA cm−2, while the symmetrical battery had a lifetime of up to 160 hours when the zinc utilization rate reached 95%. The SSZIBs could maintain a capacity of 98.61% after 720 hours of self-discharge, showing excellent stability.

4.2 Construction of component-regulated CEI

By designing the component composition of CEI, this strategy can directionally achieve properties, such as hydrophobic migration inhibition, ion sieving or side reaction suppression, avoiding the limitations of relying solely on interface structure modification.115–118 For instance, to address the issues of VO2+/VO2+ shuttling and H2O erosion in VOx cathodes, He et al. constructed a CEI with specific hydrophobic components. By adjusting the proportion of hydrophobic functional groups in the membrane, they not only blocked the cross-interface migration of VO2+ and VO2+, but also inhibited the penetration of H2O into the cathode interior.119 Miu et al. introduced strontium ions into the vanadium oxide layer as sacrificial guests. During cycling, these strontium ions precipitated from the cathode and participated in CEI formation. Through component reconstruction, the CEI was endowed with the ability to dynamically inhibit vanadium dissolution.120 This work reports a universal strategy for constructing electrode–electrolyte interfaces, providing insights into inhibiting the dissolution of vanadium-based cathodes in SSZIBs.

4.3 Self-separating interface layer

In addition to the above-mentioned directional modification strategy of artificial CEI films to cathode materials, the interface engineering is further expanding towards dynamic adaptation and multi-interface coordinated control.121–125 For example, Qiu et al. constructed an interface layer composed of sodium tricyanomethylated to evolve to form an electrically responsive shielding layer composed of nitrogen, carbon-rich polymer networks and sodium ions.126 This interface layer can not only regulate the migration pathway of Zn2+ and inhibit interface side reactions, but also shield the tip effect and induce uniform deposition. Due to the formation of a stable interface layer of cathode and electrolyte, this characteristic improves the structural stability of cathode, so that the Zn‖Zn symmetrical battery achieves excellent cycle life (3000 h) and rate performance (20 A g−1) in a wide temperature range, and the Zn‖NaV3O8·1.5H2O full battery also achieves an ultra-long life of more than 10[thin space (1/6-em)]000 circles.

5. Conclusions and outlook

SSZIBs, as promising contenders for next-generation energy storage technologies, exhibit enhanced performance that hinges crucially on thorough investigations into the optimization of the cathode–electrolyte interface. Despite recent progress in refining these interfaces in SSZIBs, three pivotal challenges continue to persist within interfacial research. Firstly, there is the issue of interface chemical stability and the management of side reactions at high potentials. Secondly, mechanical stress accumulation and ion transport dynamics challenges arise during cycling, driven by lattice alterations and mismatches in the thermal expansion coefficients of cathode materials. Thirdly, the complexity of solid–solid multiphase interfaces and the controllability of the fabrication process pose additional hurdles.

Based on this, future research on interface optimization can achieve breakthroughs through three primary technical pathways as shown in Fig. 12. For example, (1) employ cross-scale characterization techniques, including in situ characterization at the atomic level and synchrotron radiation imaging tests at the mesoscopic scale, to deeply investigate the correlation between interface microstructure and performance, thereby providing a scientific basis for precise interface design; (2) integrate machine learning technology, utilizing graph neural networks to predict and optimize the optimal interface composition, strengthen learning algorithms to develop digital models for interface failure prediction, ultimately accelerating material design, research, and development; (3) to address engineering challenges, implement strategies such as solution-based self-assembly, roll-to-roll electrospinning equipment, and the use of biodegradable interface layer materials, aimed at reducing costs, enabling large-scale production, and enhancing environmental compatibility, thereby laying a solid foundation for the industrial application of cathode materials in SSZIBs.


image file: d5ta07455j-f12.tif
Fig. 12 Research trends on cathode interfaces of future SSZIBs.

Author contributions

Yitao Zhao: literature investigation, writing-original draft. Lingbiao Meng: literature investigation. Linhong Mao: visualization, methodology. Yan Nie: conceptualization. Siyao Jiang: investigation. Guosen Zhou: visualization. Jingjing Yuan: supervision, writing-review & editing.

Conflicts of interest

There are no conflicts to declare.

Data availability

No primary research results, software or code have been included and no new data were generated or analysed as part of this review.

Acknowledgements

The authors gratefully acknowledge the financial support from Changzhou Municipal Applied Basic Research Program (No. CJ20253019, CJ20220180) and Jiangsu Provincial Science and Technology Plan Project Youth Fund (No. BK20230639).

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