Double-Network Gel-Enabled Uniform Incorporation of Metallic Matrices with Silicon Anodes Realizing Enhanced Lithium Storage

Silicon–metal (Si–M) binary materials manifest high tap densities and areal capacities and desirable Li-storage behavior benefiting from metallic matrices and thus have been regarded as promising anodic choices in next-generation Li-ion batteries. To fully realize the hybridization merits, the uniform incorporation of metallic components with silicon is a prerequisite, yet it remains a significant challenge via facile and economic routes. Herein we develop an all-inorganic, double-network, gel-enabled methodology for the uniform incorporation of metallic matrices with silicon anodes. Taking Si–Ti binary materials as an example, the simultaneous gelation reaction for both SiO2 and TiO2 gel networks ensures the formation of integrative SiO2–TiO2 double-network gels, guaranteeing the uniform incorporation of metallic titanium with nanoporous silicon framework via a subsequent magnesiothermic coreduction process. Thanks to the unique structural and compositional features, the as-prepared Si–Ti binary framework exhibits a long cycle life (1161 mA h g–1 after 100 cycles at 0.5 A g–1) and a high rate capability (1405 and 1190 mA h g–1 at 1 and 2 A g–1, respectively).