Investigation of ion-electrode interactions of linear polyimides and alkali metal ions for next generation alternative-ion batteries.
Investigation of ion-electrode interactions of linear polyimides and alkali metal ions for next generation alternative-ion batteries.
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下一代交替离子电池用线型聚醯亚胺与碱金属离子之离子-电极交互作用之研究。
DOI：
10.1039/d2sc02939a
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发表时间：
2022-08-17
期刊：
影响因子：
8.4
通讯作者：
中科院分区：
文献类型：
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作者：
有机电极材料提供了利用离子-电极相互作用来开发多样化、多功能和高性能二次电池的独特机会，特别是对于需要高功率密度的应用。然而，氧化还原活性有机材料缺乏明确的结构-性能关系限制了该领域的发展。在这里，我们研究了一个家庭的二酰亚胺基聚合物材料与几个电荷补偿离子（Li+，Na+，K+），以系统地探测如何氧化还原活性部分，离子和聚合物的灵活性决定其热力学和动力学性质。当采用有利的离子-电极相互作用时（例如，软K+阴离子与软二萘嵌苯二酰亚胺二价阴离子），所得电池显示出增加的工作电位和改善的循环稳定性。此外，对于本文检查的所有聚合物，我们证明K+由于其小的溶剂化壳/能量而获得最高百分比的氧化还原活性基团。通过冠醚实验，循环伏安法和活化能测量，我们提供了三种不同的聚合物结构的电荷补偿机制的见解，并合理化这些发现的不同程度的改善时，观察到的循环与K+。重要的是，我们发现，最灵活的聚合物能够访问最高分数的活性位点，由于在充电/放电过程中的小活化能势垒。这些结果表明，可以通过采用更灵活的结构来提高容量。总的来说，我们深入的结构-活性研究展示了聚合物结构和阳离子等变量如何用于优化电池性能，并实现新型电池化学。有机电极材料提供了利用离子-电极相互作用来开发多样化、多功能和高性能二次电池的独特机会，特别是对于需要高功率密度的应用。
Organic electrode materials offer unique opportunities to utilize ion-electrode interactions to develop diverse, versatile, and high-performing secondary batteries, particularly for applications requiring high power densities. However, a lack of well-defined structure–property relationships for redox-active organic materials restricts the advancement of the field. Herein, we investigate a family of diimide-based polymer materials with several charge-compensating ions (Li+, Na+, K+) in order to systematically probe how redox-active moiety, ion, and polymer flexibility dictate their thermodynamic and kinetic properties. When favorable ion-electrode interactions are employed (e.g., soft K+ anions with soft perylenediimide dianions), the resulting batteries demonstrate increased working potentials and improved cycling stabilities. Further, for all polymers examined herein, we demonstrate that K+ accesses the highest percentage of redox-active groups due to its small solvation shell/energy. Through crown ether experiments, cyclic voltammetry, and activation energy measurements, we provide insights into the charge compensation mechanisms of three different polymer structures and rationalize these findings in terms of the differing degrees of improvements observed when cycling with K+. Critically, we find that the most flexible polymer enables access to the highest fraction of active sites due to the small activation energy barrier during charge/discharge. These results suggest that improved capacities may be accessible by employing more flexible structures. Overall, our in-depth structure–activity investigation demonstrates how variables such as polymer structure and cation can be used to optimize battery performance and enable the realization of novel battery chemistries. Organic electrode materials offer unique opportunities to utilize ion-electrode interactions to develop diverse, versatile, and high-performing secondary batteries, particularly for applications requiring high power densities.
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影响因子：
2.2
作者：
Kaunda, Rennie B.
通讯作者：
Kaunda, Rennie B.
影响因子：
29.4
作者：
Han, Xiaoyan;Chang, Caixian;Sun, Jutang
通讯作者：
Sun, Jutang
影响因子：
5.4
作者：
Komaba, Shinichi;Hasegawa, Tatsuya;Kubota, Kei
通讯作者：
Kubota, Kei
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影响因子：
27.8
作者：
Hu, Yanyao;Gao, Yang;Lu, Bingan
通讯作者：
Lu, Bingan
影响因子：
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作者：
Andrzejak, M;Mazur, G;Petelenz, P
通讯作者：
Petelenz, P