硅材料是开发高容量锂离子电池的理想负极材料之一，但其在充放电过程的显著的体积效应导致其电化学性能衰减，制约了硅材料商业化应用。使用具有自修复功能的弹性聚合物粘结剂是缓解硅材料体积效应的有效途径。然而，新能源汽车的高速发展对锂离子电池的比容量和循环性能有更高的要求，需要硅负极在有限的时间内对电极的微裂纹有快速、充分的修复。因此，修复速度快、修复效率高的自修复聚合物粘结剂亟待开发。基于此，本项拟合成基于四重氢键相互作用的自修复超分子聚合物粘结剂聚丙烯酸-酰脲嘧啶酮（PAA-UPy），研究PAA-UPy/Si复合电极电化学储能性能，建立材料-结构-性能构效关系。通过对复合电极自修复机制的深入理解，期望本项目能够开发出得到一类比容量不低于3800mAh/g、循环200周后比容量不少于2500mAh/g的实用型高性能复合硅负极，并为设计开发新型自修复聚合物粘结剂提供新思路，促进硅负极的商业化应用。

With extremely high specific capacity, silicon has attracted enormous interests as a promising anode material for the next-generation lithium-ion battery. However, silicon suffers large volume variation during repeated charge/discharge cycles, which leads to the pulverization of silicon and subsequent separation from the conductive additives, eventually resulting in rapid capacity fading and poor cyclic life. Here we show that the utilization of a quadruple hydrogen bonding supramolecular polymer, which can be facilely synthesized by the radical copolymerization of tert-butyl acrylate and a ureido pyrimidinone (UPy) monomer followed by hydrolysis, could greatly relieve the effect of volume variation of silicon particles. The obtained polymer can consist of self-healing property as its strong quadruple hydrogen bonding. The electrodes using this supramolecular polymer as binder are expected to significantly improve of both a high capacity (>3800 mAh/g) with long cycling life (>2500 mAh/g after 200 cycles) and favorable initial columbic efficiency (>85%). Therefore, this supramolecular strategy may increase the choice of amendable binders to improve cycle lives and energy density of high-capacity Li-ion battery electrodes.