Enhancing Stability and 6C Fast Charging in µSi||LiNi0.8Co0.1Mn0.1O2 Lithium‐Ion Batteries Using Conductive Binders With Multiple Hydrogen Bonds

Abstract Micro‐sized silicon (µSi) anodes are an attractive alternative to graphite for high‐energy lithium‐ion batteries (LIBs) due to their low cost and high specific capacity. However, they suffer from severe volume expansion during lithiation, leading to fast capacity decay and poor rate capability. Herein, a new hybrid binder featuring a cross‐linked conductive network and multiple hydrogen bonds for µSi anodes with high areal capacity is reported. This binder demonstrates multi‐scale synergistic effects, including robust binder‐derived solid electrolyte interphase, multiple networks to mitigate electrode pulverization and efficient ion/electron transfer pathways. As a result, the µSi anodes exhibit long‐term cyclability and exceptional rate performance, achieving a high specific capacity of 1481.3 mAh g −1 at 12 A g −1 and maintaining 960.5 mAh g −1 at 20 A g −1 . When paired with the LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode, the µSi||NCM811 full cell delivers an impressive capacity of 145.8 mAh g −1 under fast 6C charging conditions, along with high Coulombic efficiency during cycling. This research presents an effective strategy for enabling fast charging and stable cycling in high‐energy µSi‐based LIBs.