Adina Rubella‐Like Microsized SiO@N‐Doped Carbon Grafted with N‐Doped Carbon Nanotubes as Anodes for High‐Performance Lithium Storage

Microsized silicon oxide (SiO) has become a highly potential anode material for practical lithium‐ion batteries (LIBs) in virtue of its low cost and high capacity. However, its commercialization is still impeded by the low inherent conductivity and nonignorable volume expansion of SiO in the lithiation/delithiation processes. Herein, an in situ catalytic growth approach is developed for grafting N‐doped bamboo‐like carbon nanotubes (NCNTs) onto the polydopamine‐coated SiO microparticles, yielding a unique adina rubella‐like SiO@NC‐NCNT composite. The cross‐sectional scanning electron microscopy images reveal that the flexible middle‐carbon layer plays a crucial role in alleviating volume expansions and improving structural stability of SiO@NC‐NCNTs. Theoretical density functional theory simulation results further prove that the rational construction of ternary heterostructure can effectively balance lithium adsorption energies and greatly improve conductivity of SiO@NC‐NCNTs. As a result, the as‐fabricated SiO@NC‐NCNTs LIB anode shows a high reversible specific capacity of 1103.7 mA h g −1 at 0.2 A g −1 after 200 cycles with a high retention of 99.6% and an outstanding rate capability of 569 mA h g −1 at 5000 mA g −1 . The strategy developed herein demonstrates a feasible avenue for developing high‐energy SiO‐based anodes for LIBs.