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

所有聚合物基电池都是基于聚合物阳极和阴极材料。由于其有趣的性质，如重量轻，替代关键金属的可能性和可用元素的利用，它们获得了很多兴趣。各种各样可能的分子结构已经被探索作为活性材料，导致许多氧化还原部分可用。有趣的是，与较少的合适的阳极材料相比，有更多的阴极材料可用，如多紫原。然而，这些材料也有缺点。在此背景下，耶拿FSU和吉森JLU的联合项目将开发基于三种结构基序的新型氧化还原活性聚合物-苯并咪唑，苯并恶唑和苯并噻唑-都是吡啶取代的。这些材料被证明是我们第一次利用理论和实验筛选相结合的方法中作为阳极材料的合适候选者。因此，电化学性质将通过取代基的变化而进一步调整。此外，将通过DFT的计算和理论筛选来研究合适的线性双功能分子的氧化还原部分。在确定了最有希望的结构之后，第二步是小聚合物链的建模。将合成最佳聚合物体系，并对其电化学性能进行研究。聚合物结构也将是多种多样的。第一代活性材料在侧链上具有氧化还原基团，而第二代活性材料将产生主链上具有氧化还原基团的聚合物。具有最佳电化学性能的高分子材料将被用于制造电极。这些电极将在（半）电池测试中进行测试，例如与基于tempo的聚合物结合作为阴极材料。

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.