【摘要】 自修复材料是指材料受到外力损伤后能够进行自我修复的材料。将自修复聚合物作为电解质应用于锂离子电池，能提升电池在极端环境下的安全性和稳定性。但是自修复聚合物在理论计算方面的研究较少。通过高通量计算和模拟优选具有自修复功能的聚合物电解质材料，开展了羟基、羧基、羰基、硫醇键等典型高分子链段之间的分子间作用力的理论计算（发现羰基酯键的相互作用能大于0.1 eV），并计算了羰基酯键、二硫键、硼酸酯键等动态共价键交换反应的交换活化能（分别为4.32 eV、5.78 eV和2.51 eV）及其在电解液中发生交换反应的理论温度（低于25℃）。最后根据上述计算结果，模拟了聚合物电解质在典型锂电池电解液中的自修复行为，验证了含有羰基酯键、二硫键、硼酸酯键的聚合物高分子具有良好的自修复性质。本研究可为未来高安全性电池的开发提供重要参考。更多还原

【Abstract】 Self-healing material refers to the material that can heal itself after being damaged by external forces. The application of self-healing polymers as solid polymer electrolytes in lithiumion batteries can greatly improve the safety and stability of batteries in extreme environments, thus extending their service life. However, there is little research on theoretical calculation of selfhealing polymer electrolyte. In this study, polymer electrolytes based on self-healing materials were optimized through high-throughput calculation and simulation. First, theoretical calculation of intermolecular interaction forces between typical polymer segments such as hydroxyl, carboxyl,carbonyl, mercaptan bonds was carried out. It was found that the interaction energy of ester bond was greater than 0.1 eV. Then the exchange activation energy of the exchange reaction of ester bond, disulfide bond, borate ester bond and other dynamic covalent bonds were worked out to be4.32 eV, 5.78 eV and 2.51 eV, respectively, and the theoretical temperature of exchange reaction in the electrolyte was figured out to be lower than 25 ℃. Finally, according to the above calculation results, the self-healing behavior of polymer electrolytes in typical lithium battery electrolytes was simulated. It is proved that the polymer containing carbonyl ester bond, disulfide bond and borate ester bond has good self-healing properties. The findings can provide important references for the development of high safety batteries in the future.更多还原