Silicon-Based Self-Assemblies for High Volumetric Capacity Li-Ion Batteries via Effective Stress Management

Silicon nanoparticles (Si NPs) have been considered as promising anode materials for next-generation lithium-ion batteries, but the practical issues such as mechanical structure instability and low volumetric energy density limit their development. At present, the functional energy-storing architectures based on Si NPs building blocks have been proposed to solve the adverse effects of nanostructures, but designing ideal functional architectures with excellent electrochemical performance is still a significant challenge. This study shows that the effective stress evolution management is applied for self-assembled functional architectures via cross-scale simulation and the simulated stress evolution can be a guide to design a scalable self-assembled hierarchical Si@TiO2@C (SA-SiTC) based on core-shell Si@TiO(2)nanoscale building blocks. It is found that the carbon filler and TiO(2)layer can effectively reduce the risk of cracking during (de)lithiation, ensuring the stability of the mechanical structure of SA-SiTC. The SA-SiTC electrode shows long cycling stability (842.6 mAh g(-1)after 1000 cycles at 2 A g(-1)), high volumetric capacity (174 mAh cm(-3)), high initial Coulombic efficiency (80.9%), and stable solid-electrolyte interphase (SEI) layer. This work provides insight into the development of the structural stable Si-based anodes with long cycle life and high volumetric energy density for practical energy applications.