Silicon (Si), which exhibits high theoretical capacity, is a promising material for high energy density anode material in Lithium Ion Batteries (LIBs) because it is abundant in nature, inexpensive, and eco-friendly. However, Si has excessive volume expansion with charge and discharge cycles, resulting in reduced capacity reversibility and collapsing electrode structures. To overcome this limitation, polymer binders equipped with various functions have been used to improve the electrochemical performance of Si. The present study developed a self-healing cross-linked poly(acrylic acid) (PAA) binder for Si anodes functionalized with diarylbibenzofuranone (DABBF), which exhibits self-healing from reversible C-C bonding and the debonding of dynamic carbon radicals. When applied to Si anodes, the PAA-based binder functionalized with DABBF formed a three-dimensional network, stabilizing the Si structure and achieving improved adhesion and mechanical properties. Its self-healing performance enabled the Si anodes to exhibit stable capacity retention. In addition, the adhesion performance and mechanical properties of Si anodes were higher when DABBF-functionalized PAA was used as a binder. At a current density of 0.5 C, a high initial coulombic efficiency (ICE) of 77.89% was achieved, and after 500 cycles, the capacity remained high, 1774.45 mAh g⁻¹. A novel cross-linked polymer binder with self-healing ability was successfully developed for the first time using dynamic carbon radicals, and its excellent electrochemical performance significantly improved the stability of Si anodes.

硅 (Si) 具有很高的理论容量，是锂离子电池 (LIB) 中高能量密度负极材料的有前途的材料，因为它在自然界中含量丰富、价格低廉且对环境友好。然而，随着充电和放电循环，Si 的体积膨胀过度，导致容量可逆性降低和电极结构坍塌。为了克服这一限制，具有多种功能的聚合物粘合剂已被用于改善硅的电化学性能。本研究开发了一种用于二芳基联苯并呋喃酮 (DABBF) 功能化硅阳极的自愈交联聚丙烯酸 (PAA) 粘合剂，它表现出可逆 CC 键合和动态碳自由基脱键的自愈性。当应用于硅阳极时，用 DABBF 功能化的 PAA 基粘合剂形成了三维网络，稳定了 Si 结构并提高了附着力和机械性能。其自我修复性能使硅负极能够保持稳定的容量。此外，当使用 DABBF 功能化的 PAA 作为粘合剂时，Si 负极的粘附性能和机械性能更高。在0.5 C的电流密度下，获得了77.89%的高初始库仑效率（ICE），500次循环后，容量仍然很高，为1774.45 mAh g 当DABBF功能化的PAA用作粘合剂时，硅负极的粘附性能和机械性能更高。在0.5 C的电流密度下，获得了77.89%的高初始库仑效率（ICE），500次循环后，容量仍然很高，为1774.45 mAh g 当DABBF功能化的PAA用作粘合剂时，硅负极的粘附性能和机械性能更高。在0.5 C的电流密度下，获得了77.89%的高初始库仑效率（ICE），500次循环后，容量仍然很高，为1774.45 mAh g^-1。首次利用动态碳自由基成功开发出一种具有自修复能力的新型交联聚合物粘合剂，其优异的电化学性能显着提高了硅负极的稳定性。