Optimized Pinecone-Squama-Structure MoS2-Coated CNT and Graphene Framework as Binder-Free Anode for Li-Ion Battery with High Capacity and Cycling Stability

Extensive research has been conducted on the development of high-rate and cyclic stability anodes for lithium batteries (LIBs) due to their high energy density. Molybdenum disulfide (MoS2) with layered structure has garnered significant interest due to its exceptional theoretic Li+ storage behavior as anodes (670 mA h g−1). However, achieving a high rate and long cyclic life of anode materials remains a challenge. Herein, we designed and synthesized a free-standing carbon nanotubes-graphene (CGF) foam, then presented a facile strategy to fabricate the MoS2-coated CGF self-assembly anodes with different MoS2 distributions. Such binder-free electrode possesses the advantages of both MoS2 and graphene-based materials. Through rational regulation of the ratio of MoS2, the MoS2-coated CGF with uniformly distributed MoS2 exhibits a nano pinecone-squama-like structure that can accommodate the large volume change during the cycle process, thereby significantly enhancing the cycling stability (417 mA h g−1 after 1000 cycles), ideal rate performance, and high pseudocapacitive behavior (with a 76.6% contribution at 1 mV s−1). Such a neat nano-pinecone structure can effectively coordinate MoS2 and carbon framework, providing valuable insights for the construction of advanced anode materials.