Development of active materials for organic batteries based on electropolymerized polymers equipped with stable organic radicals

今天的电池技术主要基于金属，如锂、铅、钴或镍。然而，它们有限的自然存在以及它们的毒性和由此产生的处置问题限制了它们的可用性。或者，可以使用聚合物化合物。在此背景下，基于稳定有机自由基的聚合物被深入研究，揭示了有希望的电荷存储性能，特别是优越的氧化还原反应动力学。然而，这种材料的导电性差，这限制了适用的充电/放电速率，取消了有利的电子转移特性。克服这个问题的一个有希望的方法是结合导电，即共轭聚合物。这些材料提供了几个可以用于有机电池的有益特性：(1)作为半导体，它们具有导电性；（ii）它们可以通过电聚合应用，提供了一种直接在电极表面制备不溶性聚合物结构的有效方法；（三）它们本身提供电荷存储能力。虽然共轭聚合物的存储能力往往受到倾斜的充放电电压的限制，但电导率和电化学可加工性与稳定的氧化还原部分（如有机自由基）相结合，呈现出非常有利的特征。根据最近的研究结果，该项目的重点在于提高所建器件的长期稳定性和电子导电性。这一目标将通过综合计算方法中所涉及的分子构建块的变化来实现。因此，通过电化学聚合制备的含有稳定有机自由基和共轭聚合物的全有机电池构成了最终目标。

Today's battery technology is mostly based on metals, such as lithium, lead, cobalt, or nickel. However, their limited natural occurrence as well as their toxicity and the resulting disposal problems limit their usability. Alternatively, polymeric compounds can be used. In this context, polymers based on stable organic radicals were studied intensively revealing promising charge-storage properties, in particular a superior redox reaction kinetic. However, such materials suffer from poor electrical conductivity, which limits the applicable charging/discharging rates, cancelling the advantageous electron-transfer characteristic. A promising approach to overcome this problem is the incorporation of conductive, i.e., conjugated, polymers. These materials offer several beneficial features that can be exploited for an organic battery: (i) As semiconductors, they offer electronical conductivity; (ii) they can be applied via electropolymerization, offering an efficient way to prepare insoluble polymeric structures directly on an electrode surface; and (iii) they themselves offer charge-storage capability. While the storage capability of conjugated polymers is often restricted due to a sloping charge / discharge voltage, the electronical conductivity as well as the electrochemical processability present highly advantageous features in combination with a stable redox moiety such as organic radicals. Based on recent results, the focus of the project lies on the improvement of the long-term stability and electronic conductivity of the built devices. This goal shall be realized by the variation of the involved molecular building blocks within a combined synthetic-computational approach. Consequently, an all-organic battery containing stable organic radicals and conjugated polymers prepared by means of electrochemical polymerization constitutes the final target.