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Lithium-ion batteries with high energy density and long cycle life have been widely used as secondary batteries in electric vehicles and energy storage systems. With the growing demand for high energy density in lithium-ion batteries, silicon-based materials, which possess a high theoretical specific capacity (4200 mAh g−1), are regarded as core candidates for anode materials. However, Si-based materials undergo severe volume expansion (up to 300%), which leads to the collapse of the electrode structure, inducing pulverization of the active material and capacity loss, thereby hindering the commercial application of silicon-based materials. To address these issues, scholars from various countries have developed many silicon-based materials with different compositions and three-dimensional structures, and have made some research progress. This review first elaborates on the lithium storage mechanisms and advantages of diverse silicon-based anode materials by taking Si, SiOx, SiNx, and SiPx as representative examples with distinct characteristics. Subsequently, from the two aspects of dimensional design (0D, 1D, 2D and 3D) and architecture design (core–shell, sandwich-like and network structure), the design strategies for various silicon-based anode structures and their enhancement on electrochemical performance are analyzed. Finally, this review elucidated the challenges faced by silicon-based anodes from the perspectives of mechanism elucidation, structural customization, industrialization, and full-cell applications. It also proposed future development directions for silicon anodes by combining actual challenges and focusing on aspects such as structure optimization, machine learning, advanced characterization techniques, and mechanistic analysis.
Wu et al. (Mon,) studied this question.