Silicon‐Based Lithium Ion Battery Systems: State‐of‐the‐Art from Half and Full Cell Viewpoint

Lithium‐ion batteries (LIBs) have been occupying the dominant position in energy storage devices. Over the past 30 years, silicon (Si)‐based materials are the most promising alternatives for graphite as LIB anodes due to their high theoretical capacities and low operating voltages. Nevertheless, their extensive volume changes in battery operation causes the structural collapse of Si‐based electrodes, as well as severe side reactions. In this review, the preparation methods and structure optimizations of Si‐based materials are highlighted, as well as their applications in half and full cells. Meanwhile, the developments of promising electrolytes, binders and separators that match Si‐based electrodes in half and full cells have made great progress. Pre‐lithiation technology has been introduced to compensate for irreversible Li+ consumption during battery operation, thereby improving the energy densities and lifetime of Si‐based full cells. More importantly, almost all related mechanisms of Si‐based electrodes in half and full cells are summarized in detail. It is expected to provide a comprehensive insight on how to develop high‐performance Si‐based full cells. The work can help us understand what happens during the lithiation process, the primary causes of Si‐based half and full cells failure, and strategies to overcome these challenges. Promising Si‐based batteries should have outstanding and balanced performance between energy density and lifetime. Specifically, the development of cathodes, the modification of Si anodes, electrolytes, binders, and separators, as well as state of the art pre‐lithiation technologies are critical to facilitate the practical application of Si‐based batteries.