With the rapid development of advanced energy storage equipment, particularly lithium-ion batteries (LIBs), there is a growing demand for enhanced battery energy density across various fields. Consequently, an increasing number of high-specific-capacity cathode and anode materials are being rapidly developed. Concurrently, challenges pertaining to insufficient battery safety and stability arising from liquid electrolytes (LEs) with flammability persistently emerge. LEs possess the advantages of exceptional ionic conductivity and can operate within a broader temperature range. After two decades of continuous development in commercial applications, it currently stands as the most widely employed electrolyte material in lithium-ion batteries. However, the existing LE primarily consists of a carbonate electrolyte with a low flash point, low boiling point, and flammable and volatile nature, thereby rendering fire and explosion risks inevitable. Compared with LEs, solid-state electrolytes (SSEs) exhibit relatively good flame retardancy and possess the potential to inhibit lithium dendrite formation, and they are regarded as promising electrolyte materials. Nevertheless, numerous challenges of SSEs still need to be addressed at this stage. The inadequate solid–solid contact between the solid electrolyte and the electrode material, as well as the insufficient contact stability, significantly impact the cycling stability of solid-state batteries. Furthermore, unlike liquid electrolytes, the solid electrolyte lacks fluidity and cannot effectively penetrate the pores of porous electrodes, necessitating additional cathode design considerations. The incompatibility with existing liquid battery production processes and high cost further impede the advancement of solid-state batteries. In response to the challenges associated with solid-state batteries, recent research has introduced in situ solidification solutions. By transformation of the liquid into a solid electrolyte within the battery, this method facilitates excellent interfacial contact between the electrolyte and electrode material while ensuring compatibility with existing production equipment. Consequently, these advantages have propelled in situ solidification to become a prominent research methodology for solid-state batteries. Currently, electrolyte research is undergoing a transitional period from liquid to solid-state, accompanying the emergence of numerous hybrid solid–liquid electrolytes (HSLEs). HSLEs not only exhibit the high ionic conductivity characteristic of liquid electrolytes but also enhance battery safety and stability to a certain extent. HSLEs are found in various forms, including hybrid systems comprising inorganic solid electrolytes and LEs, as well as gel systems consisting of polymer electrolytes and LEs. Additionally, there are in situ solidification technologies that enable the gel electrolyte to be formed internally within the battery. This concept introduces the development status of electrolytes with improved safety and stability from the perspectives of LEs, SSEs, and HSLEs.

中文翻译：

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用于可充电锂金属电池的先进电解质，具有高安全性和循环稳定性

随着先进储能设备特别是锂离子电池（LIB）的快速发展，各个领域对提高电池能量密度的需求日益增长。因此，越来越多的高比容量正极和负极材料正在迅速开发。与此同时，易燃液体电解质（LE）带来的电池安全性和稳定性不足的挑战持续出现。LE 具有出色的离子电导率的优点，并且可以在更广泛的温度范围内工作。经过二十年的商业应用不断发展，目前已成为锂离子电池中应用最广泛的电解质材料。然而，现有的电解液主要由碳酸盐电解质组成，具有低闪点、低沸点、易燃易挥发等特点，不可避免地存在着火和爆炸的风险。与LE相比，固态电解质（SSE）表现出相对良好的阻燃性，并具有抑制锂枝晶形成的潜力，被认为是有前途的电解质材料。尽管如此，现阶段上证所仍面临诸多挑战需要解决。固体电解质与电极材料之间的固-固接触不充分以及接触稳定性不足，显着影响固态电池的循环稳定性。此外，与液体电解质不同，固体电解质缺乏流动性，无法有效渗透多孔电极的孔隙，因此需要额外的阴极设计考虑。与现有液态电池生产工艺的不兼容以及高成本进一步阻碍了固态电池的进步。为了应对与固态电池相关的挑战，最近的研究引入了原位固化解决方案。通过在电池内将​​液体转化为固体电解质，该方法有利于电解质和电极材料之间良好的界面接触，同时确保与现有生产设备的兼容性。因此，这些优点推动原位固化成为固态电池的重要研究方法。目前，电解质研究正经历从液态到固态的过渡期，伴随着众多混合固液电解质（HSLE）的出现。HSLE不仅表现出液体电解质的高离子电导率特性，而且在一定程度上增强了电池的安全性和稳定性。HSLE有多种形式，包括由无机固体电解质和LE组成的混合系统，以及由聚合物电解质和LE组成的凝胶系统。此外，还有原位固化技术，可以在电池内部形成凝胶电解质。