Accurately Localizing Multiple Nanoparticles in a Multishelled Matrix Through Shell‐to‐Core Evolution for Maximizing Energy‐Storage Capability

Abstract Robust and fast lithium energy storage with a high energy density is highly desired to accelerate the market adoption of electric vehicles. To realize such a goal requires the development of electrode materials with a high capacity, however, such electrode materials suffer from huge volume expansion and induced short cycling life. Here, using tin (Sn) as an example, an ideal structure is designed to effectively solve these problems by separately localizing multiple Sn nanoparticles in a nitrogen‐doped carbon hollow multishelled structure with duplicated layers for carbon shell (Sn NPs@N_xC HoMS‐DL). The fabricated composite can promote ion and electron diffusion owing to the conductive network formed by connected multiple shells and cores, effectively buffer the volume expansion, and maintain a stable electrode–electrolyte interface. Despite the challenging fabrication, such a structure is realized through an innovative and facile synthesis strategy of “in situ evolution of shell to core”, which is applicable for diverse low‐melting‐point materials. As expected, such a structure enables the high‐capacity electrode material to realize nearly its theoretical lithium‐storage capability: the developed Sn NPs@N_xC HoMS‐DL electrode maintains 96% of its theoretical capacity after 2000 cycles at 2C.