Organosilicon‐Based Functional Electrolytes for High‐Performance Lithium Batteries

The electrolyte has been considered as a key factor toward higher energy density for Li‐ion and Li‐metal batteries. However, conventional electrolytes suffer from uncontrolled interfacial reactions and irreversible decomposition causing performance deterioration and potential safety hazard. Organosilicon compounds have attracted great interest as promising electrolyte components due to facile chemical modifications, low glass transition temperatures (Tg), superior chemical, and thermal stabilities. Considerable investigation efforts have been devoted to developing better overall performance of organosilicon‐based electrolytes in the past few years. Herein, the recent research progress of organosilicon‐based functional electrolytes for the development of liquid, gel, and solid state electrolytes in Li‐ion and Li‐metal batteries is summarized. Attention is devoted to various types of organosilicon such as silane, siloxane, polysiloxane, and polyhedral oligomeric silsesquioxanes in terms of molecular design, ionic conductivity, functions shown in batteries, thermal, chemical, electrochemical stability, safety, etc. The feasible strategies are also discussed that may promote the comprehensive electrochemical performances of organosilicon‐based electrolytes in different types of electrolytes and batteries. Finally, the challenges facing organosilicon‐based electrolytes and proposed their possible solutions are presented alongside promising development directions. The development of organosilicon functional electrolytes including silane, siloxane, polysiloxane, and polyhedral oligomeric silsesquioxanes are systematically summarized and discussed in terms of high‐voltage, safety, and thermal stability for lithium batteries. The strategies are also indentified that could meet the current challenges and the future directions of organosilicon functional electrolytes for electrochemical energy storage.