High-Toughness and Hierarchical Stress-Dissipating Binder Based on Physicochemical Dual-Cross-Linking for High-Performance Silicon Anodes

• DOI: 10.1021/acsami.4c22696
• Publication Date: 2025-04-01T05:30:19Z
• Authors: Yang He; Feng Zhou; Yingxi Zhang; Tuan Lv; Paul K. Chu; Kaifu Huo

Silicon (Si) is a promising anode material for next-generation lithium-ion batteries (LIBs), but the huge volume change of Si particles causes fracture and delamination from current collector, thereby stifling practical implementation. Herein, high-toughness hierarchical stress-dissipating binder anodes prepared by covalent hydrogen bonding poly(acrylic acid) (PAA) cross-linked polyurethane (CPU). The physicochemical dual-cross-linked CPU-PAA with high toughness, large tensile strength, stress dissipation improves structural integrity minimizes thickness swelling. Finite element analysis confirms that reduces uniformizes distribution within during cycling. As result, Si/CPU-PAA shows capacity retention 82.3% after 150 cycles at density 5 A g–1. Moreover, Si/CPU-PAA//LiNi0.5Co0.2Mn0.3O2 full cell delivers stable cycling performance, highlighting great potential in high-energy-density LIBs. This work provides insights into design high-strength, large-toughness, efficient binders high-performance anodes.