Benzoquinone-Based Polyimide Derivatives as High-Capacity and Stable Organic Cathodes for Lithium-Ion Batteries
Benzoquinone-Based Polyimide Derivatives as High-Capacity and Stable Organic Cathodes for Lithium-Ion Batteries
复制标题
苯醌基聚酰亚胺衍生物作为锂离子电池的高容量且稳定的有机正极
DOI：
10.1021/acsami.9b18422
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发表时间：
2020-01-08
影响因子：
9.5
通讯作者：
Zhao, Xin
中科院分区：
文献类型：
--
作者：
Ba, Zhaohu;Wang, Zhengxing;Zhao, Xin
通过Michael加成反应合成了一种含苯醌单元的新型二胺单体，并与二酐进行了面缩聚反应，合成了多羰基聚酰亚胺衍生物。苯醌和二酐的羰基与苯胺结构键的巧妙结合不仅提供了每个单元具有大量羰基的稳定聚合物链，而且还保证了其大π共轭主链，这有利于其长循环寿命和快速动力学。当用作锂离子电池正极材料时，基于萘二酸酐的聚酰亚胺衍生物在0.1C下的可逆比容量为145 mAh/g，在1C下的高倍率性能为108 mAh/g，并且在0.5C下的1000次循环后具有超长稳定的循环性能，容量保持率为80.3%。基于理论计算和电化学行为的探索，对制备样品的可逆离子插入反应提出了合理的预测，以深入理解电荷存储机制。此外，在醚基电解质中形成的稳定的固体电解质界面膜被证实改善了电化学性能。
Multicarbonyl polyimide derivatives were synthesized by a facial condensation polymerization of dianhydrides with a new diamine monomer containing a benzoquinone unit that was prepared according to the Michael addition reaction. The ingenious combination of dedicated carbonyl groups from the benzoquinone and dianhydride with an aniline structure linkage not only provided stable polymeric chains with a high number of carbonyl groups per unit but also guaranteed their large pi-conjugated main chains, which is favorable to their long cycle life and fast kinetics. When explored as cathode materials for lithium-ion batteries, the polyimide derivatives based on naphthalic dianhydride delivered a reversible specific capacity of 145 mAh/g at 0.1 C, a high rate performance with a capacity of 108 mAh/g at 1 C, and an ultralong stable cyclic performance with a capacity retention of 80.3% after 1000 cycles at 0.5 C. Based on the theoretical calculations and the exploration of the electrochemical behaviors, sensible predictions for the reversible ion-insertion reaction of the as-prepared sample were proposed to deeply understand the charge storage mechanisms. Moreover, a stable solid electrolyte interphase film formed in the ether-based electrolyte was confirmed to improve the electrochemical properties.