Built-in konjac gum molecular adhesive for stress-adaptive interlocked silicon anodes

Structural rational design and efficient preparation are the key to improve the sluggish electrode kinetics and mitigate volume changes during electrochemical process for Si-based anodes. Nano carbons with good electronic, ionic conductivity and mechanical properties have been adopted to improve the performance of Si anodes. However, the interface bonding between nano carbons and Si particles is not strong enough to form good electron conduction channels and lithium-ion diffusion pathways. Herein, this work designed a rGO@KG@CNTs@Si composite anodes for Lithium-ion batteries through low-dimensional topology assembly with carbon nanotubes (CNTs), reduced graphene oxide (rGO), integrate konjac gum (KG) and Si particles as building blocks. The preparation involves a gelation and molecular self-assembly process to integrate KG as an inbuilt adhesive. The introduction of CNTs can interweave and intertwine to form an interlocking structure, which not only serves as 1D novel conductors to improve the electrode conductivity, but also supports the 2D rGO layers to prevent their stacking. This structural feature could enhance the electrochemical performance and decrease the expansion stress of Si. The rGO@KG@CNTs@Si-3 electrode exhibited a remarkable capacity retention of 2004 mAh/g after 100 cycles, with low interfacial resistance and rapid lithium-ion transfer. Mechanisms were elucidated through in-situ electrochemical impedance spectroscopy, distribution of relaxation time and multi-scale molecular modeling calculations. These findings offer a scalable solution for constructing stable, high-performing anodes, advancing next-generation Lithium-ion batteries development.