Structural Design and Challenges of Micron‐Scale Silicon‐Based Lithium‐ion Batteries

Abstract Currently, lithium‐ion batteries (LIBs) are at the forefront of energy storage technologies. Silicon‐based anodes, with their high capacity and low cost, present a promising alternative to traditional graphite anodes in LIBs, offering the potential for substantial improvements in energy density. However, the significant volumetric changes that silicon‐based anodes undergo during charge and discharge cycles can lead to structural degradation. Furthermore, the formation of excessive solid‐electrolyte interphases (SEIs) during cycling impedes the efficient migration of ions and electrons. This comprehensive review focuses on the structural design and optimization of micron‐scale silicon‐based anodes from both materials and systems perspectives. Significant progress is made in the development of advanced electrolytes, binders, and conductive additives that complement micron‐scale silicon‐based anodes in both half and full‐cells. Moreover, advancements in system‐level technologies, such as pre‐lithiation techniques to mitigate irreversible Li + loss, have enhanced the energy density and lifespan of micron‐scale silicon‐based full cells. This review concludes with a detailed classification of the underlying mechanisms, providing a comprehensive summary to guide the development of high‐energy‐density devices. It also offers strategic insights to address the challenges associated with the large‐scale deployment of silicon‐based LIBs.