Electrostatic Interactions Leading to Hierarchical Interpenetrating Electroconductive Networks in Silicon Anodes for Fast Lithium Storage

Abstract Recently, the frequency of combining MXene, which has unique properties such as metal‐level conductivity and large specific surface area, with silicon to achieve excellent electrochemical performance has increased considerably. There is no doubt that the introduction of MXene can improve the conductivity of silicon and the cycling stability of electrodes after elaborate structure design. However, most exhaustive contacts can only improve the electrode conductivity on the plane. Herein, a MXene@Si/CNTs (HIEN‐MSC) composite with hierarchical interpenetrating electroconductive networks has been synthesized by electrostatic self‐assembly. In this process, the CNTs are first combined with silicon nanoparticles and then assembled with MXene nanosheets. Inserting CNTs into silicon nanoparticles can not only reduce the latter‘s agglomeration, but also immobilizes them on the three‐dimensional conductive framework composed of CNTs and MXene nanosheets. Therefore, the HIEN‐MSC electrode shows superior rate performance (high reversible capacity of 280 mA h −1 even tested at 10 A g −1 ), cycling stability (stable reversible capacity of 547 mA h g −1 after 200 cycles at 1 A g −1 ) and applicability (a high reversible capacity of 101 mA h g −1 after 50 cycles when assembled with NCM622 into a full cell). These results may provide new insights for other electrodes with excellent rate performance and long‐cycle stability.