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

By Xiaoming Zhou, Yang Liu, Yang Ren, Tiansheng Mu, Xucai Yin, C. Du, Hua Huo, Xinqun Cheng, Pengjian Zuo, Geping Yin. Advanced Functional Materials, 2021

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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 (<5 nm) in carbon hollow capsids at a nanocluster scale. The obtained SiOx/C hollow spheres exhibit excellent Li+‐ion storage behaviors, including cycling lifespan, coulombic efficiency, and rate performance. The superior performance is attributed to the well‐dispersed SiOx nanoclusters in carbon substrate and the hollow structure. This molecular polymerization approach not only enables Si‐based hollow composites effective and scalable anode materials but also opens up a new avenue for the controllable synthesis of template‐free hollow architectures.

Subfields: Electrical and Electronic Engineering, Electronic, Optical and Magnetic Materials

View Paper: https://www.semanticscholar.org/paper/63ceeb642934be9ece8514844bd1e80d1cdb49b0