Hydrogen Bond-Interlocked Conductive Polymeric Networks with Integrated Rigidity and Flexibility: Empowering the Stable Functioning of Silicon–Carbon Anodes

The commercial application of silicon–carbon microparticles (Si/C) as anode materials in advanced high-energy-density lithium-ion batteries (LIBs) has been hindered by suboptimal interfacial stability and insufficient cycling durability, which are primarily attributed to the detrimental stress generated during the lithiation and delithiation processes. In this study, a polymeric binder (PTR) was developed for Si/C anodes in lithium-ion batteries. The PTR binder was fabricated by integrating rigid poly(acrylic acid) (PAA) with flexible carboxylated styrene–butadiene rubber (XSBR) through cross-linking with tannic acid (TA), thereby forming a stable molecular architecture. Additionally, carboxylated single-wall carbon nanotubes (SWCNTs) were incorporated to construct a dual cross-linking conductive network. This unique design effectively alleviates the stress induced by silicon expansion, suppresses chain slippage, and maintains the structural integrity of the electrode. Electrochemical tests demonstrated that Si/C anodes employing the PTR binder exhibited significantly enhanced capacity retention and rate performance in comparison to those utilizing traditional binders. This research offers a promising strategy for improving the structural stability and electrochemical performance of Si/C anodes, thereby facilitating the advancement of high-energy-density LIBs.