The desirable specific theoretical capacity (3579 mAh g⁻¹) of silicon (Si) renders it beneficial as a next-generation anode for lithium-ion batteries (LIBs). However, the significant volume expansion restricts its commercial application. Here, inspired by natural Boston ivy, an efficient and facile strategy to design a three-dimensional (3D)-crosslinked binder for high-performance Si-based anodes enabled by synergizing “Disk” (small molecules) and “Vine” (long chains) is reported. The small molecule branch-like tannic acid (TA) rich in hydroxyl (−OH) groups tends to have multidimensional hydrogen-bonding interactions with the Si surfaces. Meanwhile, the long chains of polysaccharides, such as carboxymethyl cellulose (CMC) and hyaluronic acid (HA), are beneficial for the large-scale bridging of components in an electrode. Moreover, the in-situ cross-linking of TA and polysaccharides can establish a 3D network to release the inner stress of Si particles. Consequently, this cooperation benefits stable slurry, high adhesive strength, and favorable rate performance. Moreover, when over 100 cycles, the Si anode incorporating tannic-carboxymethyl cellulose (TAC) as the binder delivers a high specific capacity of 2782 mAh g⁻¹. Additionally, favorable practicality is demonstrated by the stable operation of a commercial silicon/graphite (Si/Gr) anode and full-cells.

理想的比理论容量（3579 mAh g ^-1) 的硅 (Si) 使其有利于作为锂离子电池 (LIB) 的下一代阳极。然而，显着的体积膨胀限制了其商业应用。在这里，受天然波士顿常春藤的启发，一种高效简便的策略可以通过协同“Disk”（小分子）和“Vine”（长链）来设计用于高性能硅基阳极的三维 (3D) 交联粘合剂) 报道。富含羟基 (-OH) 的小分子支链状单宁酸 (TA) 倾向于与 Si 表面发生多维氢键相互作用。同时，长链多糖，如羧甲基纤维素（CMC）和透明质酸（HA），有利于电极中组分的大规模桥接。而且，TA和多糖的原位交联可以建立3D网络以释放Si颗粒的内应力。因此，这种合作有利于稳定浆料、高粘合强度和良好的倍率性能。此外，当循环次数超过 100 次时，以单宁羧甲基纤维素 (TAC) 作为粘合剂的硅负极可提供 2782 mAh g 的高比容量^-1。此外，商用硅/石墨 (Si/Gr) 阳极和全电池的稳定运行证明了良好的实用性。