Hybrid crosslinking for in-situ encapsulation of three-dimensional porous SiOx@rGO as high-performance anodes in lithium-ion batteries

Abstract

Silicon suboxide (SiOx) anodes have garnered significant attention from both academia and industry due to their superior theoretical capacity compared to graphite, as well as their improved capacity retention in comparison to pure silicon. Nevertheless, SiOx electrodes still confront the challenge of substantial volume expansion (>160 %) during the alloying process, resulting in electrode structural damage or even fragmentation and severely impacting cycling performance. Here, a three-dimensional (3D) conductive network was constructed by ethylenediamine (EDA) cross-linking reduced graphene oxide (rGO), which was encapsulated on the surface of SiOx spheres generated in situ via a magnesium thermal reduction reaction. Accordingly, the SiOx@rGO-EDA anode was prepared successfully with high reversible capacity (892 mAh g−1 after 100 cycles at 1 A g−1) and fascinating rate performance (447 mAh g−1 at 4 A g−1). In full cell, the SiOx@rGO-EDA anode also exhibits outstanding cycling stability (154 mAh g−1 after 100 cycles at 0.1C) and rate capability. The scanning electron microscopy (SEM) images captured from a top-view perspective indicate that the surface of SiOx@rGO-EDA electrode is smooth and dense without any noticeable cracks, and it maintains its structural integrity throughout the cycling process. The cross-sectional thickness of the electrode remains essentially the same. These results illustrate the superior structural stability of the EDA cross-linked graphene conductive network cladding structure, enabling it to adapt to dynamic changes and ensure efficient transport of lithium ions and electrons. The facile and versatile synthesis method of SiOx@rGO-EDA structures by incorporating cross-linking agents provides inspiration for the design of next-generation high-performance anodes.