Interfacial nitrogen engineering of robust silicon/MXene anode toward high energy solid-state lithium-ion batteries

Replacing the conventional carbonate electrolyte by solid-state electrolyte (SSE) will offer improved safety for lithium-ion batteries.To further improve the energy density,Silicon (Si) is attractive for next generation solid-state battery (SSB) because of its high specific capacity and low cost.High energy density and safe Si-based SSB,however,is plagued by large volume change that leads to poor mechanical stability and slow lithium ions transportation at the multiple interfaces between Si and SSE.Herein,we designed a self-integrated and monolithic Si/two dimensional layered T_(3)C_(2)T_(x)(MXene,T_(x) stands for terminal functional groups) electrode architecture with interfacial nitrogen engineering.During a heat treatment process,the polyacrylonitrile not only converts into amorphous carbon (a-C) that shells Si but also forms robust interfacial nitrogen chemical bonds that anchors Si and MXene.During repeated lithiation and delithiation processes,the robust interfacial engineered Si/MXene configuration enhances the mechanical adhesion between Si and MXene that improves the structure stability but also contributes to form stable solid-electrolyte interphase (SEI).In addition,the N-MXene provides fast lithium ions transportation pathways.Consequently,the Si/MXene with interfacial nitrogen engineering (denoted as Si-N-MXene) deliveres high-rate performance with a specific capacity of 1498 m Ah g^(-1) at a high current of 6.4 A g^(-1).A Si-N-MXene/NMC full cell exhibited a capacity retention of 80.5%after 200 cycles.The Si-N-MXene electrode is also applied to SSB and shows a relative stable cycling over 100 cycles,demonstrating the versatility of this concept.