Rechargeable batteries, typically represented by lithium-ion batteries, have taken a huge leap in energy density over the last two decades. However, they still face material/chemical challenges in ensuring safety and long service life at temperatures beyond the optimum range, primarily due to the chemical/electrochemical instabilities of conventional liquid electrolytes against aggressive electrode reactions and temperature variation. In this regard, a gel polymer electrolyte (GPE) with its liquid components immobilized and stabilized by a solid matrix, capable of retaining almost all the advantageous natures of the liquid electrolytes and circumventing the interfacial issues that exist in the all-solid-state electrolytes, is of great significance to realize rechargeable batteries with extended working temperature range. We begin this review with the main challenges faced in the development of GPEs, based on extensive literature research and our practical experience. Then, a significant section is dedicated to the requirements and design principles of GPEs for wide-temperature applications, with special attention paid to the feasibility, cost, and environmental impact. Next, the research progress of GPEs is thoroughly reviewed according to the strategies applied. In the end, we outline some prospects of GPEs related to innovations in material sciences, advanced characterizations, artificial intelligence, and environmental impact analysis, hoping to spark new research activities that ultimately bring us a step closer to realizing wide-temperature rechargeable batteries.

Gel polymer electrolytes for rechargeable batteries toward wide-temperature applications.

All-solid-state batteries (ASSBs) have garnered significant interest due to their exceptional safety features and high theoretical energy density. Despite extensive research demonstrating the impressive electrochemical performance of ASSBs at moderate and high temperatures, their electrochemical performance significantly degrades in a cold environment, with the underlying mechanism yet to be disclosed. In this review, we examine the ion transport kinetics of ASSBs and emphasize the challenges they face at low temperatures. By examining microscopic kinetic processes, including Li-ion migration within solid electrolytes (SEs), interfacial charge transfer, and bulk electrode diffusion, we outline the critical challenges and specific requirements on SEs, interfaces, and electrodes for low-temperature ASSBs. Based on these insights, a range of materials and chemistry design strategies for high-performance ASSBs at low temperatures are reviewed. Finally, future research directions for improving low-temperature ASSB performance are proposed. This study aims to offer a thorough understanding and crucial insights to improve the low-temperature performance of ASSBs. 

Materials and chemistry design for low-temperature all-solid-state batteries

All‐solid‐state lithium batteries (ASSLBs) are considered a promising technology for next‐generation energy storage systems due to their inherent safety. However, the conventional laboratory‐scale ASSLBs reported to date are based on pellet‐type structures with thick solid electrolyte layers, leading to challenges related to low energy densities and poor electrochemical performance. In this study, porous adhesive poly(ethylene vinyl acetate) (PEVA) scaffolds and polytetrafluoroethylene (PTFE) binders are utilized to interweave sulfide solid electrolytes into freestanding films with an ultra‐low thickness of 40 µm, high ionic conductivity of 1.1 mS cm−1, and a high tensile strength of 74 MPa. To mitigate the reduction reaction between the PTFE binder and the lithium metal anode, a Li3N‐rich solid electrolyte interphase (SEI) in situ on lithium metal is formed, and the assembled symmetric cell shows excellent cycling stability within 800 h at the current density of 0.2 mA cm−2 and room temperature. Additionally, the ASSLBs using oxidatively stable Li2ZrCl5F in the composite cathode and the prepared solid electrolyte film demonstrate exceptional cycling performance and fast‐charging capability, with a high cell‐level energy density of 354.4 Wh kg−1. The ASSLBs prepared by coupling E‐LPSCl film and stable interface design exhibit excellent electrochemical performance and a high cell‐level energy density.

High Ionic Conductive, Mechanical Robust Sulfide Solid Electrolyte Films and Interface Design for All‐Solid‐State Lithium Metal Batteries

All-solid-state batteries (ASSBs) have attracted considerable attention due to their theoretically high energy density and safety. However, maintaining intimate interfacial contact at low external pressures remains a challenge, limiting large-scale practical applications. Here, a bottom-up design of all-solid-state electrodes is proposed by minimizing internal stress variation to maintain interfacial transport at low external pressures. Theoretical calculations and synchrotron X-ray techniques reveal that the surface-to-bulk pillar effect alleviates the volumetric strain of the cathode materials at high delithiation, which is favorable for improving the interfacial mechanical and chemical compatibility to create fast ion percolation networks of the electrode. Therefore, the 4.4 V sulfide-based ASSBs retain a high specific capacity (166.7 mAh g–1, 0.2C), good rate performance, and stable cyclability (90.8% retention) at the operating pressure of 2 MPa. This work sheds light on the design concept of electrochemomechanical manipulation, serving as a guideline for developing practically acceptable low-pressure ASSBs. 

Maintaining Interfacial Transports for Sulfide-Based All-Solid-State Batteries Operating at Low External Pressure

Applying high stack pressure (often up to tens of megapascals) to solid-state Li-ion batteries is primarily done to address the issues of internal voids formation and subsequent Li-ion transport blockage within the solid electrode due to volume changes. Whereas, redundant pressurizing devices lower the energy density of batteries and raise the cost. Herein, a mechanical optimization strategy involving elastic electrolyte is proposed for SSBs operating without external pressurizing, but relying solely on the built-in pressure of cells. We combine soft-rigid dual monomer copolymer with deep eutectic mixture to design an elastic solid electrolyte, which exhibits not only high stretchability and deformation recovery capability but also high room-temperature Li-ion conductivity of 2×10-3 S cm-1 and nonflammability. The micron-sized Si anode without additional stack pressure, paired with the elastic electrolyte, exhibits exceptional stability for 300 cycles with 90.8% capacity retention. Furthermore, the solid Li/elastic electrolyte/LiFePO4 battery delivers 143.3 mAh g-1 after 400 cycles. Finally, the micron-sized Si/elastic electrolyte/LiFePO4 full cell operates stably for 100 cycles in the absence of any additional pressure, maintaining a capacity retention rate of 98.3%. This significantly advances the practical applications of solid-state batteries. 

A solid-state lithium-ion battery with micron-sized silicon anode operating free from external pressure

Realizing long-cycling all-solid-state Li-In||TiS2 batteries using Li6+xMxAs1-xS5I (M=Si, Sn) sulfide solid electrolytes

The development of all-solid-state lithium-metal batteries (ASSLMB) has long been impeded by low coulomb efficiency, short lifetime, poor rate performance and other problems caused by the rapid growth of lithium (Li) dendrites. Herein, a multiple-diffusion-channel N,S-doped soft carbon with expanded layer spacing was designed/developed by thiourea calcination for dendrite-free anodes. Since the enlarged layer spacing can improve Li+ transportation rate within the layers and N,S-doping can facilitate Li+ transport between the layers, the bulk phase diffusion (not just surface diffusion) kinetics can be improved, which in turn reduces the local current density, inhibits the growth of Li dendrites, and improves the rate performance. The resulting ASSLMB achieves record-high current density (15 mA cm-2 ), areal capacity (20 mAh cm-2 ), energy density (403 Wh kg-1 ), and ultra-long cycle life (13,000 cycles). >305 Wh kg-1 pouch cells were realized, representing one of the most critical breakthroughs for real-world application of ASSLMBs. This article is protected by copyright. All rights reserved.

Soft Carbon-Thiourea With Fast Bulk Diffusion Kinetics For Solid-State Lithium Metal Batteries.

The rapid growth of lithium (Li) dendrites has long hindered the development of all‐solid‐state lithium‐metal batteries (ASSLMB). Here, a composite soft carbon (SC)‐nano Si3N4 (SiN) interlayer (SC‐SiN) is designed for in situ formation of Li3N network (with high ionic conductivity/diffusivity) after lithium embedding in nano‐Si3N4, promoting the rapid migration of Li+ and guiding the metal Li to be deposited uniformly in a 3D manner within the interlayer. It can solve the problem of rapid consumption of Li+ and local charge accumulation at the interface of solid electrolyte and Li metal anode, thus avoiding the growth of Li‐dendrites. The resulting LCO/LPSCl/SC‐SiN‐Li ASSLMB achieves ultra‐high current density (12.5 mA cm−2) and ultra‐long cycle life (22 000 cycles with no degradation), as well as ultra‐high area capacity area capacity (15 mAh cm−2) and energy density (402.5 Wh kg−1), all of which break existing ASSLMB records. In addition, it is capable of 600 cycles at an areal capacity of 2.7 mAh cm−2 and 2 C (85.7% capacity retention). A pouch cell is also assembled to delivers high energy density (>320 Wh kg−1). These confirm the application potential of this configuration and are one of the most critical breakthroughs toward the commercialization of the ASSLMB.

In Situ Formed Li3N Networks by Soft Carbon‐Si3N4 for Superior All‐Solid‐State Lithium‐Metal Batteries

New insight into efficient photocatalytic CO2 reduction without any sacrifice agent over the novel hierarchical structured SiOC whisker aerogel

Ion transport in solids is a key topic in solid-state ionics. It is critical but challenging to understand the relationship between material structures and ion transport. Nanochannels in crystals provide ion transport pathways, which are responsible for the fast ion transport in fast lithium (Li)-ion conductors. The controlled synthesis of carbon nanotubes (CNTs) provides a promising approach to artificially regulating nanochannels. Herein, the CNTs with a diameter of 5.5 Å are predicted to exhibit an ultralow Li-ion diffusion barrier of about 10 meV, much lower than those in routine solid electrolyte materials. Such a characteristic is attributed to the similar chemical environment of a Li ion during its diffusion based on atomic and electronic structure analyses. The concerted diffusion of Li ions ensures high ionic conductivities of CNTs. These results not only reveal the immense potential of CNTs for fast Li-ion transport but also provide a new understanding for rationally designing solid materials with high ionic conductivities.

Diameter-dependent ultrafast lithium-ion transport in carbon nanotubes.

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