Spider Silk‐Inspired Binder Design for Flexible Lithium‐Ion Battery with High Durability

Abstract The development of flexible lithium‐ion batteries (LIBs) imposes demands on energy density and high mechanical durability simultaneously. Due to the limited deformability of electrodes, as well as the flat and smooth surface of the metal current collectors, stable/durable/reliable contact between electrode materials and the current collectors remains a challenge, in particular, for electrodes with high loading mass and heavily deformed batteries. Binders play an essential role in binding particles of electrode materials and adhering them to current collectors. Herein, inspired by spider silk, a binder for flexible LIBs is developed, which equips a cross‐linked supramolecular poly(urethane‐urea) to the polyacrylic acid. The binder imparts super high elastic restorability originating from the meticulously engineered hydrogen‐bonding segments as well as extraordinary adhesion. The developed binder provides excellent flexibility and intact electrode morphologies without disintegration even when the electrode is largely deformed, enabling a stable cycling and voltage output even when the batteries are put under tough dynamic deformation tests. The flexible LIBs exhibit a high energy density of 420 Wh L⁻¹, which is remarkably higher than reported numbers. The unique binder design is greatly promising and offers a valuable material solution for LIBs with high‐loading mass and flexible designs.