Development of novel redox-active polymers based on benzimidazole, benzoxazole and benzothiazole

所有基于聚合物的电池都是基于聚合物负极和阴极材料。由于它们具有重量轻、可替代关键金属和可利用可利用元素等有趣的性质，因此引起了人们的极大兴趣。人们探索了许多可能的分子结构作为活性物质，导致了许多氧化还原部分的出现。有趣的是，与更少的合适的阳极材料相比，有更多的阴极材料可用，比如聚紫精。然而，这些材料也存在缺陷。在这方面，FSU Jena和JLU Giessen的这一联合项目将基于三个结构基元--苯并咪唑、苯并恶唑和苯并噻唑--开发新的氧化还原活性聚合物，这些结构基元都是吡啶取代的。在我们首次采用理论和实验相结合的方法中，这些材料被证明是合适的负极候选材料。因此，取代基的变化将进一步调整其电化学性质。此外，还将通过密度泛函理论的计算和筛选来研究线型双功能分子的合适氧化还原基团。在确定了最有希望的结构之后，第二步是对小聚合物链进行建模。将合成最佳的聚合物体系，并研究它们的电化学性质。聚合物结构也将多种多样。第一代活性物质的氧化还原部分位于侧链，第二代活性物质的氧化还原部分位于主链。具有最佳电化学性能的聚合物材料将被用于电极的制造。这些电极将在(半)电池测试中进行测试，例如与以TEMPO为基础的聚合物组合作为阴极材料。

All polymer-based batteries are based on polymeric anode as well as cathode materials. Due to their interesting properties, such as light-weight, the possibility to replace critical metals and the utilization of available elements, they have gained much interest. A large variety of possible molecular structures has been explored as active materials, resulting in many redox moieties being available. Interestingly, there is a larger number of cathode materials being available compared to fewer suitable anode materials, like the polyviologens. However, also these materials suffer from drawbacks. In this context, this joint project of the FSU Jena and the JLU Giessen will develop new redox-active polymers based on three structural motifs – benzimidazoles, benzoxazoles and benzothiazoles – which are all pyridyl-substituted. These materials proved to be suitable candidates as anode materials in our first combined approach utilizing theoretical and experimental screening. Consequently, the electrochemical properties will be further tuned by variation of the substituents. Furthermore, suitable redox moieties of linear bifunctional molecules will be investigated by the calculation and theoretical screening by DFT. After identification of the most promising structures, the second step is the modelling of small polymer chains. The best polymer systems will be synthesized and their electrochemical properties will be studied. The polymer architecture will also be varied. Whereas the first generation of active materials have the redox moieties in the side chain, the second generation will result in polymers with the redox moiety in the main chain. Polymeric materials with the best electrochemical properties will be used for the fabrication of electrodes. These electrodes will be tested in (half)-cell tests, for example in combination with TEMPO-based polymers as cathode materials.