Organic material holds immense potential for Li-ion batteries (LIBs) due to their eco-friendly nature, high structural designability, abundant sources, and high theoretical capacity. However, the limited redox-active sites, low electronic conductivity, sluggish ionic diffusion, and high solubility hinder their practical application. Here, we reported the use of a linear polymer called poly(naphthalenetetracarboxylic dianhydride-pyrene-4,5,9,10-tetraone)-coated graphene nanosheets (NPT/rGO) as a cathode material for LIBs. The NPT polymer has a rotation angle of approximately 63° between each plane, which helps in exposing the active sites and preventing structural pulverization during cycling. The highly conjugated skeleton of the polymer, along with graphene, forms a synergistic effect through a π–π interaction. This combination enhances the conductivity and restricts solubility. Additionally, the linear structure of NPT and the two-dimensional rGO substrates work together to enhance charge transfer and ion diffusion rates, resulting in faster reaction kinetics. Consequently, NPT/rGO exhibits excellent electrochemical performance in terms of high capacity, superior cyclic stability, and good rate capability for LIBs. Moreover, through the combination of experimental investigations and theoretical simulations, a multiple electron reaction mechanism, an efficient Li-ion storage behavior, and a reversible dynamic evolution have been revealed. This study introduces a rational molecular design approach to enhance the electrochemical performance of polyimide derivatives, thereby contributing to the advancement of cutting-edge organic electrode materials for LIBs.

中文翻译：

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具有π共轭结构和多活性中心的线性聚合物涂覆石墨烯纳米片的设计，具有长寿命和高倍率的锂存储性能


有机材料由于其环保性、结构可设计性高、来源丰富和理论容量高，在锂离子电池（LIB）方面具有巨大的潜力。然而，有限的氧化还原活性位点、低电子电导率、缓慢的离子扩散和高溶解度阻碍了它们的实际应用。在这里，我们报道了使用一种称为聚（萘四甲酸二酐-芘-4,5,9,10-四酮）涂覆的石墨烯纳米片（NPT/rGO）的线性聚合物作为LIB的阴极材料。 NPT聚合物每个平面之间的旋转角约为63°，这有助于暴露活性位点并防止循环过程中结构粉碎。聚合物的高度共轭骨架与石墨烯通过π-π相互作用形成协同效应。这种组合增强了电导率并限制了溶解度。此外，NPT 的线性结构和二维 rGO 基板共同提高电荷转移和离子扩散速率，从而实现更快的反应动力学。因此，NPT/rGO 在高容量、优异的循环稳定性和良好的锂离子电池倍率性能方面表现出优异的电化学性能。此外，通过实验研究和理论模拟相结合，揭示了多电子反应机制、高效的锂离子存储行为和可逆动态演化。这项研究引入了一种合理的分子设计方法来增强聚酰亚胺衍生物的电化学性能，从而有助于先进的锂离子电池有机电极材料的进步。