通过调节活性位密度、可及性和反应性,为锂有机电池开发高性能聚酰亚胺正极材料

IF 42.9 Q1 ELECTROCHEMISTRY eScience Pub Date : 2024-08-01 DOI:10.1016/j.esci.2023.100224
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摘要

有机羰基电极材料因其理论容量高、资源可持续性和结构多样性,为未来的储能系统提供了广阔的前景。虽然高性能羰基电极材料的研究取得了很大进展,但对影响其电化学性能的基本因素的系统深入研究却相当有限。本文设计并合成了五种含有不同类型二胺连接体的聚酰亚胺作为锂离子电池的阴极材料。首先,在共轭和非共轭体系中,羰基的加入都会增加活性位密度。其次,增加分子刚性可提高活性位点的可及性。第三,在两个羰基之间引入共轭结构可以提高活性位点的反应活性。因此,羰基结构和共轭结构的加入提高了聚酰亚胺的容量。在 50 mA g-1 的条件下,PTN、PAN、PMN、PSN 和 PBN 的电容量分别为 212、198、199、151 和 115 mAh g-1。此外,引入羰基结构和共轭结构也有利于提高循环稳定性和速率性能。这项工作可以加深对结构-功能关系的理解,从而合理设计聚酰亚胺电极材料,并可扩展到其他有机阴极材料的分子设计。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Towards high performance polyimide cathode materials for lithium–organic batteries by regulating active-site density, accessibility, and reactivity

Organic carbonyl electrode materials offer promising prospects for future energy storage systems due to their high theoretical capacity, resource sustainability, and structural diversity. Although much progress has been made in the research of high-performance carbonyl electrode materials, systematic and in-depth studies on the underlying factors affecting their electrochemical properties are rather limited. Herein, five polyimides containing different types of diamine linkers are designed and synthesized as cathode materials for Li-ion batteries. First, the incorporation of carbonyl groups increases the active-site density in both conjugated and non-conjugated systems. Second, increased molecular rigidity can improve the accessibility of the active sites. Third, the introduction of the conjugated structure between two carbonyl groups can increase the reactivity of the active sites. Consequently, the incorporation of carbonyl structures and conjugated structures increases the capacity of polyimides. PTN, PAN, PMN, PSN, and PBN exhibit 212, 198, 199, 151, and 115 ​mAh ​g−1 ​at 50 ​mA ​g−1, respectively. In addition, the introduction of a carbonyl structure and a conjugated structure is also beneficial for improving cycling stability and rate performance. This work can deepen the understanding of the structure–function relationship for the rational design of polyimide electrode materials and can be extended to the molecular design of other organic cathode materials.

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