As the need for new modalities of energy storage becomes increasingly important, all-solid-state secondary ion batteries seem poised to address a portion of tomorrow’s energy needs. The success of such batteries is contingent on the solid-state electrolyte (SSE) meeting a set of material demands, including high bulk and interfacial ionic conductivity, processability with electrodes, electrode interfacial stability, thermal stability, etc. The demanding criteria for an ideal SSE has translated into decades of research devoted to discovering new electrolytes and modifying their structure/processing to improve their properties. While much research has focused on the electrolyte properties of polycrystalline ceramics, non-crystalline materials (glasses, amorphous solids, and partially crystallized materials) have demonstrated unique advantages in processability, stability, tunability, etc. These non-crystalline electrolytes are also fundamentally interesting for their potential contributions toward understanding ionic conduction in the solid state. In this review, we first review a decade of advances in two distinct families of non-crystalline lithium-ion electrolytes: lithium thiophosphate and lithium phosphate oxynitride. In doing so, we demonstrate two pathways for non-crystalline electrolytes to address the barriers toward development of all-solid-state batteries, viz., interfacial stability and conduction. Finally, we conclude with some discussion of the development of fundamental models of ionic conduction in the non-crystalline state, including the ongoing debate between strong and weak electrolyte theories. Collectively, these discussions make a promising case for the role of non-crystalline electrolytes in the next generation of energy storage technology.

随着对新的能量存储方式的需求变得越来越重要，全固态二次离子电池似乎已准备好解决明天的部分能源需求。此类电池的成功取决于固态电解质（SSE）是否满足一系列材料要求，包括高体积和界面离子电导率，带电极的可加工性，电极界面稳定性，热稳定性等。理想的苛刻标准SSE已转化为数十年的研究，致力于发现新的电解质并修改其结构/工艺以改善其性能。尽管许多研究都集中在多晶陶瓷，非晶体材料（玻璃，无定形固体，以及部分结晶的材料）在加工性，稳定性，可调性等方面已显示出独特的优势。这些非晶态电解质从根本上也引起了人们的兴趣，因为它们对于理解固态的离子传导具有潜在的贡献。在这篇综述中，我们首先回顾了两种不同的非晶体锂离子电解质家族的十年进展：硫代磷酸锂和磷酸锂氧氮化物。这样做，我们证明了非晶态电解质解决全固态电池发展障碍的两种途径，即界面稳定性和导电性。最后，我们讨论了非晶态离子传导基本模型的发展，包括强电解质理论和弱电解质理论之间正在进行的辩论。总而言之，这些讨论为非晶态电解质在下一代储能技术中的作用提供了有希望的案例。