Abstract
Silicon (Si) is a promising candidate for high‐capacity anode materials owing to its high theoretical capacity (3579 mAh g−1), low working voltage, and wide natural abundance, although its huge volume variation during charge/discharge processes always results in a short cycling life. Polymer binders play a vital role in improving the cycling performance of Si‐based anodes, although traditional polyvinylidene difluoride cannot fulfil the requirements owing to its weak van der Waals forces with the Si surface. Recently, polymer binders constructed by dynamic bonds have been developed, which are reported to allow high‐energy‐density electrodes with improved electrochemical performance. With dynamic bonds including hydrogen bonding, ionic bonding, and host–guest interactions, these polymer binders possess self‐healing capabilities and enhanced mechanical performance, achieving a tremendous advance in addressing the capacity fading of Si‐based anodes. In this review, we will summarize the research progress of polymer binders constructed with dynamic bonds, and the challenges for their real applications in advanced Li‐ion batteries will also be discussed.