A Novel Gelatin Binder with Helical Crosslinked Network for High‐Performance Si Anodes in Lithium‐Ion Batteries

Abstract Silicon (Si) is a promising anode material for lithium‐ion batteries, but its large volume expansion during cycling poses a challenge for the binder design. In this study, a novel gelatin binder is designed and prepared with a helical crosslinked network structure. This gelatin binder is prepared by enzymatic crosslinking and immersion in Hofmeister salt solution, which induces the formation of network and helical secondary structures. The helical crosslinked network structure can be analogous to a spring group system to effectively dissipate the stress and strain caused by the Si expansion. The gelatin binder is further partially carbonized by low‐temperature pyrolysis, which improves its conductivity and stability. The Si anode with the optimized gelatin binder exhibits high initial coulombic efficiency, excellent rate performance, and long‐term cycling stability. This study provides an innovative approach for the preparation of high‐performance Si anodes, namely by controlling the molecular configuration of the binder to significantly improve the cycle stability, which can also be applied to other high‐capacity anode materials that suffer from large volume changes during cycling.