Synthesis of graphene-siloxene nanosheet based layered composite materials by tuning its interface chemistry: An efficient anode with overwhelming electrochemical performances for lithium-ion batteries

Abstract Owing to its high theoretical storage capacity, two dimensional (2D) silicon nanosheets is the one among the most exciting anode material for the next generation lithium ion (Li-ion) batteries. However, deprived electrochemical properties due to the huge volume expansion resulting in rapid capacity decay, thereby hindering its commercial application aspect of silicon nanosheet based materials. The present work proposes a novel concept of synthesizing graphene-siloxene (SiG) based multi-layered structures by tuning the interface chemistries of graphene oxide and siloxene sheets derived from topochemical transformation of calcium silicide (CaSi2). Morphological characterization using Field emission scanning electron microscopic and transmission electron microscopy reveal the successful formation of few- to multi-layered SiG composite materials with intercalated/surface grafted siloxene nanosheets on the graphene layers. Owing to its hierarchical composite structure, SiG as anode delivers the first discharge and charge capacity values as high as 3880 mAhg−1 and 3016 mAhg−1 respectively measured at the current rate of 205 mAg−1. Even at high current rate (4.1 Ag-1), SiG composite materials delivers first charge capacity of 1480 mAhg−1 with good cycling performance (1040 mAhg−1) after 1000 cycles. Due to its enhanced lithium storage, cycling stability and rate capability, synthesized SiG composites could be a potential anode candidate for Li-ion batteries.