Engineering Molecular Polymerization for Template‐Free SiOx/C Hollow Spheres as Ultrastable Anodes in Lithium‐Ion Batteries

SiOx/C composites with a void‐reserving structure are promising anodes for lithium‐ion batteries. However, the facile and controllable synthesis of uniformly dispersed SiOx and carbon components, simultaneously incorporating ample voids, still remains a great challenge. Herein, a molecular polymerization strategy is devised to construct SiOx/C hollow particles for lithium‐ion batteries. 3‐aminopropyltriethoxysilane and dialdehyde molecules are judiciously engineered as silicon and carbon precursors to produce the polymer hollow spheres (PHSs) through a one‐step aldimine condensation without any template and additive. A range of PHSs is obtained using terephthalaldehyde, glutaraldehyde, and glyoxal as the crosslinkers, demonstrating the high tunability of the strategy. Importantly, in situ pyrolysis of the PHSs warrants the homogeneous incorporation of SiOx (