Emerging inorganic amorphous solid-state electrolytes in all-solid-state lithium batteries: From crystallographic order to atomic and lattice disorder

Solid-state electrolytes (SEs) are the “blood vessels” in all-solid-state batteries (ASSBs), providing essential ion channels. In past decades, SE design has been mainly carried out within ordered crystalline frameworks, which is understandable for achieving well-defined ion transport pathways. However, the large impedance, poor interfaces, and dendrite penetration brought about by polycrystalline grain boundaries have always been the inherent drawbacks of crystalline SEs. Recently, tailoring disorder in crystalline SEs to achieve local atomic disorder or amorphous-state lattice disorder has emerged as an interesting strategy. In this review, we outline the working mechanism of disorder in SEs and highlight the prospects for amorphous solid electrolytes (ASEs) in advanced ASSBs, especially low-temperature ASSBs. From atomic disorder to lattice disorder, we discuss in depth the disorder-induced ion-conduction mechanism as well as properties, applications, and preparation methods. An interesting ASE closed-loop design and prediction framework is provided to meet the requirements for future ASSBs. After presenting these insights, we offer our view on the future development of ASEs.