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To enhance the compatibility between the polymer‐based electrolytes and electrodes, and promote the interfacial ion conduction, a novel approach to engineer the interfaces between all‐solid‐state composite polymer electrolyte and electrodes using thin layers of ferroelectrics is introduced. The well‐designed and ferroelectric‐engineered composite polymer electrolyte demonstrates an attractive ionic conductivity of 7.9 × 10–5 S cm–1 at room temperature. Furthermore, the ferroelectric engineering is able to effectively suppress the growth of solid electrolyte interphase (SEI) at the interface between polymer electrolytes and Na metal electrodes, and it can also enhance the ion diffusion across the electrolyte‐ferroelectric‐cathode/anode interfaces. Notably, an extraordinarily high discharge capacity of 160.3 mAh g–1, with 97.4% in retention, is achieved in the ferroelectric‐engineered all‐solid‐state Na metal cell after 165 cycles at room temperature. Moreover, outstanding stability is demonstrated that a high discharge capacity retention of 86.0% is achieved over 180 full charge/discharge cycles, even though the cell has been aged for 2 months. This work provides new insights in enhancing the long‐cyclability and stability of solid‐state rechargeable batteries. The bottleneck limiting the cyclic performance and long‐term stability of solid‐state batteries has changed from the ion conduction of electrolyte itself to electrolyte‐electrode interfaces. Herein, this issue is addressed via ferroelectric engineering at the electrolyte‐electrode interfaces. A high reversible capacity of 160.3 mAh g−1 with a retention of 97.4% is demonstrated in this all‐solid‐state Na metal cell after 165 cycles at room temperature.

Lithium metal solid‐state batteries (LMSBs) have attracted extensive attention over the past decades, due to their fascinating advantages of safety and potential for high energy density. Solid‐state electrolytes (SEs) with fast ionic transport and excellent stability are indispensable components in LMSBs. Heretofore, a series of inorganic SEs have been extensively explored, such as sulfide‐ and oxide‐based electrolytes. Unfortunately, they both have difficulty in achieving a satisfactory balance of conductivity and stability, and oxides suffer from a high impedance of grain boundaries, while sulfides encounter poor stability. Halide‐based solid electrolytes are gradually emerging as one of the most promising candidates for LMSBs due to their advantages of decent room temperature ionic conductivity (>10−3 S cm−1), good compatibility with oxide cathode materials, good chemical stability, and scalability. Herein, research and development of the widely studied metal halide SEs including fluorides, chlorides, bromides, and iodides are reviewed, mainly focusing on the structures and ionic conductivities as well as preparation methods and electrochemical/chemical stabilities. And then, based on typical metal halide solid electrolytes, we emphasize the interface issues (grain boundaries, cathode−electrolyte and electrolyte–anode interfaces) that exist in the corresponding LMSBs and summarize the related work on understanding and engineering these interfaces. Furthermore, the typical (or in situ) characterization tools widely used for solid‐state interfaces are reviewed. Finally, a perspective on the future direction for developing high‐performance LMSBs based on the halide electrolyte family is put out. The crystal structures and ionic conductivities for widely studied metal halide solid electrolytes, as well as their synthesis methods and electrochemical/chemical stabilities, are systematically summarized, with a special focus on the interface issues that exist in the corresponding lithium metal solid‐state batteries. Furthermore, the typical characterization tools widely used for solid‐state interfaces and some in situ experimental characterizations are reviewed.

This review article delves into the development of electrolytes for flexible zinc-air batteries (FZABs), a critical component driving the advancement of flexible electronics. We started by surveying the current advancements in electrolyte technologies, including solid-state and gel-based types, and their contributions to enhance the flexibility, efficiency, and durability of FZABs. Secondly, we explored the challenges in this domain, focusing on maintaining electrolyte stability under mechanical stress, ensuring compatibility with flexible substrates, optimizing ion conductivity, and under harsh environmental conditions. Furthermore, the key issues regarding interface details between electrolyte and the electrodes are covered as well. We then discussed the future of electrolyte development in FZABs, highlighting potential avenues such as materials development, sustainability, in-situ studies, and battery integration. This review offers an in-depth overview of the advancements, challenges, and potential breakthroughs in creating electrolytes for FZABs over the past five years. It serves as a guide for both researchers and industry professionals in this dynamic area.

Solid‐state lithium metal batteries are considered to be the next generation of energy storage systems due to the high energy density brought by the use of metal lithium anode and the safety features brought by the use of solid electrolytes (SEs). Unfortunately, besides the safety features, using SEs brings issues of interfacial contact of lithium anode and electrolytes. Recently, to realize the application of solid‐state lithium metal batteries, significant achievements have been made in the interface engineering of solid‐state batteries, and various new strategies have been proposed. In this review, from the interface failure perspective of solid‐state lithium metal batteries, we summarize failure mechanisms in terms of poor physical contact, weak chemical/electrochemical stability, continuing contact degradation, and uncontrollable lithium deposition. We then focused on the latest strategies for solving interface issues, including advancing in improving the physical solid–solid contact, increasing the electrochemical/chemical stability, restraining continuing contact degradation, and controlling homogeneous lithium deposition. The ultimate and paramount future developing directions of solid‐state lithium metal battery interface engineering are proposed. The failure mechanisms of the anode–electrolyte interface of solid‐state batteries include poor physical contact, weak chemical/electrochemical stability, sustained contact degradation, and uncontrolled lithium deposition. And the latest strategies to solve these interface problems include improving the solid–solid physical contact, enhancing the electrochemical/chemical stability, suppressing the sustained contact degradation, and controlling the uniform deposition of lithium.

Rechargeable batteries have been indispensable for various portable devices, electric vehicles, and energy storage stations. The operation of rechargeable batteries at low temperatures has been challenging due to increasing electrolyte viscosity and rising electrode resistance, which lead to sluggish ion transfer and large voltage hysteresis. Advanced electrolyte design and feasible electrode engineering to achieve desirable performance at low temperatures are crucial for the practical application of rechargeable batteries. Herein, the failure mechanism of the batteries at low temperature is discussed in detail from atomic perspectives, and deep insights on the solvent–solvent, solvent–ion, and ion–ion interactions in the electrolytes at low temperatures are provided. The evolution of electrode interfaces is discussed in detail. The electrochemical reactions of the electrodes at low temperatures are elucidated, and the approaches to accelerate the internal ion diffusion kinetics of the electrodes are highlighted. This review aims to deepen the understanding of the working mechanism of low‐temperature batteries at the atomic scale to shed light on the future development of low‐temperature rechargeable batteries. Low‐temperature performance of rechargeable batteries is crucial for their practical applications. This review comprehensively reveals the challenges and solutions for low‐temperature aqueous and non‐aqueous rechargeable batteries from an atomic perspective, deep insights on the solvent–solvent, solvent–ion, and ion–ion interactions in the electrolytes are provided, recent advances in the rational design of electrolytes, interfaces, and electrodes are included.

Zinc-anode batteries are known for their high capacity and safety; however, the formation of dendrites has been a concern due to their adverse effect on cycle performance. In this study, we focused on the initial formation of dendrites and performed in situ measurements using surface-sensitive grazing-incidence x-ray diffraction measurement to evaluate the atomic structure at the electrode/electrolyte interface. During the 1st charge, the zinc was deposited in an orientation close to that of the electrode; however, during the 2nd charge after the 1st discharge, it was observed that non-oriented precipitation occurred and that the surface irregularities expanded. During the discharge, it was observed that the zinc was rotating and melting, suggesting that the zinc concentration near the zinc surface decreases, making it easier to dissolve at the root of the initial dendrite than at the tip. Therefore, we suggest that future zinc-anode battery research should focus on additives that promote mass transport to dissolve the initial dendrites from their tips. Graphical Abstract

Electron tomography is an observation technique for nanometer-scale three-dimensional structures, using transmission electron microscopy (TEM). TEM tomography has been used to examine the 3D structures of various materials, such as biological samples and catalysts. In this study, we applied TEM tomography to battery materials. All-solid-state lithium-ion batteries have recently received much attention owing to their thermal safety. In all-solid-state cells, the electrode layer is composed of nonflammable solid electrolytes and electrode active materials. In order to improve the charge–discharge cycle performance, it is necessary that the electrolyte–electrode interface has no void spaces or defects. We used TEM tomography to investigate the solid interfaces of Sn–Li 3 PS 4 (LPS) negative electrode composites of all-solid-state cells. We observed that Sn, Li-Sn alloy nanoparticles, and LPS glass electrolytes formed a solid interfacial contact with no void spaces during initial charge–discharge cycles. We suggest that as a new cycle deterioration analysis method, TEM tomography is useful in evaluating solid interfaces in all-solid-state cells.

This article addresses the issue of bulk electrode design and the factors limiting the performance of thick electrodes. Indeed, one of the challenges for achieving improved performance in electrochemical energy storage devices (batteries or supercapacitors) is the maximization of the ratio between active and non-active components while maintaining ionic and electronic conductivity of the assembly. In this study, we developed and compared supercapacitor thick electrodes using commercially available carbons and utilising conventional, easily scalable methods such as spray coating and freeze-casting. We also compared different binders and conductive carbons to develop thick electrodes and analysed factors that determine the performance of such thick electrodes, such as porosity and tortuosity. The spray-coated electrodes showed high areal capacitances of 1428 mF cm−2 at 0.3 mm thickness and 2459 F cm−2 at 0.6 mm thickness.

Solid‐state sodium batteries (SSSBs) are poised to replace lithium‐ion batteries as viable alternatives for energy storage systems owing to their high safety and reliability, abundance of raw material, and low costs. However, as the core constituent of SSSBs, solid‐state electrolytes (SSEs) with low ionic conductivities at room temperature (RT) and unstable interfaces with electrodes hinder the development of SSSBs. Recently, composite SSEs (CSSEs), which inherit the desirable properties of two phases, high RT ionic conductivity, and high interfacial stability, have emerged as viable alternatives; however, their governing mechanism remains unclear. In this review, we summarize the recent research progress of CSSEs, classified into inorganic–inorganic, polymer–polymer, and inorganic–polymer types, and discuss their structure–property relationship in detail. Moreover, the CSSE–electrode interface issues and effective strategies to promote intimate and stable interfaces are summarized. Finally, the trends in the design of CSSEs and CSSE–electrode interfaces are presented, along with the future development prospects of high‐performance SSSBs. Solid‐state sodium batteries are recognized as the most promising substitute for current energy systems due to their high safety and low cost. Numerous studies on the structural design and interface engineering of solid‐state electrolytes aim to solve the critical problems in solid‐state batteries. This review summarizes the latest progress in solid‐state sodium batteries and provides insights into the design directions.