Constructing Asymmetric SiOx/C Janus Structures with Diverse Carbon Density Frameworks Enables Electrochemical Stability

Abstract The main challenges limiting the practical application of silicon‐based anode materials are volume fluctuations during cycling and poor intrinsic conductivity. One of the most effective strategies to address these limitations is the incorporation of carbon materials into silicon composites. However, few studies have investigated the impact of diverse carbon density frameworks on electrochemical performance, primarily due to the challenges associated with structural construction. Herein, an anisotropic nucleation and growth strategy is employed to control the nucleation behavior of the organosilane on the surface of nanospheres by modulating the hydrolysis environment, successfully constructing asymmetric SiO x /C Janus structures with diverse carbon density frameworks, including the assembly of the nanosphere region (BSC) with cubic‐ and rod‐shaped regions (ESC). The nucleation and growth mechanisms of the ESC region are also investigated. The exploration of the Janus structure reveals that the BSC region has a denser carbon framework, while the ESC region exhibits a sparse carbon framework. Electrochemical performance confirms that the SiO x /C anode material with a dense carbon framework exhibits superior electrochemical behavior, maintaining a capacity of 464.4 mA h g −1 after 500 cycles. Among them, the porous structure and uniform carbon frameworks of SiO x /C Janus materials contribute to both structural and electrochemical stability.