ABSTRACT The practical implementation of silicon anodes is hindered by interfacial instability and limited cycling durability, primarily due to significant volume changes and associated mechanical stresses during operation. To address these challenges, we present a stress‐dissipating binder (PAA/Cβ‐CD@TA) that utilizes the reversible boat‐chair conformational transitions of carbonyl‐β‐cyclodextrin (Cβ‐CD) to effectively dissipate stress and reduce intensity. The host‐guest interactions between tannic acid (TA) and poly(acrylic acid) (PAA) form mechanically interlocked networks, enhancing stability. Notably, the recognition between the pyrogallol groups of TA and the Cβ‐CD cavity facilitates the conversion of localized stress into reversible elastic deformation, significantly suppressing damage accumulation. This structure endows the binder with unprecedented mechanical properties, exhibiting 38.26 fold higher toughness than linear PAA, a 480 MPa reduction in Young's modulus, and 2.29 fold enhanced adhesion strength. As a result, it demonstrates exceptional electrochemical performance, retaining 73.32% capacity after 300 cycles at 4.0 A g −1 , with an initial Coulombic efficiency of 88.99% for pure silicon anodes. For commercial silicon/carbon systems, it achieves 82.25% and 75.27% capacity retention over 500 cycles at 1.0 and 2.0 C, respectively. This study provides fundamental insights into the conformational transitions of binders for stress dissipation and establishes a new paradigm for designing next‐generation silicon‐based anodes.
Jia et al. (Wed,) studied this question.