Optimized Pinecone-Squama-Structure MoS₂-Coated CNT and Graphene Framework as Binder-Free Anode for Li-Ion Battery...

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.