Benzotriazinyl radical containing polymers as bipolar active electrode material in organic secondary batteries

含有苯并三嗪基的聚合物作为有机二次电池中的双极性活性电极材料

• 批准号: 328403339
• 负责人: Professor Dr. Ulrich S. Schubert
• 金额: --
• 依托单位: Institut für Organische Chemie und Makromolekulare Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2016
• 资助国家: 德国
• 起止时间: 2015-12-31 至 2020-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/328403339?language=en
• 关键词: Benzotriazinyl; radical; containing; polymers; bipolar

The growing interest in mobile devices and their increasing integration into the World Wide Web (Internet of Things) necessitates the availability and development of small and flexible energy-storage systems. However, lithium ion batteries, which represent the current benchmark technology, do not allow the assembly of flexible batteries and demand environmentally questionable techniques for production and processing of raw materials as well as for the final disposal of disused devices. Hence, current research focuses more and more on thin film batteries that are based on organic redox active molecules, which are prepared through organic synthesis and disposed free of residues via burning. Furthermore, their (electro)chemical properties can be easily tuned through choosing a suitable chemical structure. Unfortunately, small molecules tend to dissolve in the used electrolyte leading to a significantly decreased lifetime of the battery. Thus, the monomeric redox active units are integrated into long chain polymers, which possess a substantially decreased solubility.In the course of the project, in particular polymers that are based on the benzo-1,2,4-triazinyl radical are developed. This molecule features electrochemical reversibility, high stability against air and moisture, as well as facile synthetic accessibility. Its redox characteristics can be, furthermore, easily tuned through the molecular substitution pattern, which enables even the preparation of systems that can serve both as anode and cathode material, allowing the construction of bipolar, i. e. poleless, batteries.The increase of the batteries still low theoretical capacity (from around 60 to over 100 mAh g-1) represents a central goal, which should be mainly achieved through the reduction of the molar mass of the monomer. (Electro)chemical stability, cell voltages of around 1.2 V (to allow for aqueous electrolytes), and polymerizability of the molecule have to be maintained, which is ensured through the investigation of structure-property relationships in the course of substituent variations to enable a systematic optimization of the system. The characterization process comprises the preliminary characterization of the monomeric and polymeric compounds in solution and in the solid state, the processing of the polymers with conductive additives and binder materials toward thin film composite electrodes and their subsequent characterization, as well as the assembly and comprehensive investigation of half-organic (using lithium or sodium as anode material) and full organic cells. Furthermore, the preparation of the batteries is optimized, in particular with regard to the used additives and the thin-film processing (doctor blading, inkjet printing).

人们对移动设备日益增长的兴趣以及它们与万维网（物联网）的日益融合，要求小型灵活的储能系统的可用性和开发。然而，代表当前基准技术的锂离子电池不允许组装柔性电池，并且需要对原材料的生产和加工以及废弃设备的最终处置有环境问题的技术。因此，目前的研究越来越关注基于有机氧化还原活性分子的薄膜电池，这些分子通过有机合成制备并通过燃烧无残留物处理。此外，通过选择合适的化学结构，它们的（电）化学性质可以很容易地调整。不幸的是，小分子往往会溶解在使用过的电解液中，导致电池寿命显著降低。因此，单体氧化还原活性单元被整合到长链聚合物中，其溶解度大大降低。在项目过程中，特别是基于苯并-1,2,4-三嗪基自由基的聚合物被开发出来。该分子具有电化学可逆性、对空气和水分的高稳定性以及易于合成的特点。此外，它的氧化还原特性可以很容易地通过分子取代模式进行调整，这甚至可以制备既可以作为阳极材料又可以作为阴极材料的系统，从而允许构建双极，即无极电池。提高电池的理论容量仍然很低（从大约60毫安时到100毫安时以上）代表了一个中心目标，这应该主要通过减少单体的摩尔质量来实现。（电）化学稳定性、1.2 V左右的电池电压（允许水电解质）和分子的可聚合性必须保持，这是通过研究取代基变化过程中的结构-性质关系来确保的，从而实现系统的优化。表征过程包括单体和聚合物化合物在溶液和固体状态下的初步表征，聚合物与导电添加剂和粘结材料对薄膜复合电极的加工及其后续表征，以及半有机（使用锂或钠作为阳极材料）和全有机电池的组装和全面研究。此外，优化了电池的制备，特别是关于所使用的添加剂和薄膜加工（医生叶片，喷墨打印）。

项目成果

Blatter radical as a polymeric active material in organic batteries

• DOI: 10.1016/j.jpowsour.2022.231061
• 发表时间: 2022-03
• 期刊: Journal of Power Sources
• 影响因子: 9.2
• 作者: Adrian Saal;C. Friebe;U. Schubert

Polymeric Blatter's Radical via CuAAC and ROMP

聚合布拉特的自由基通过 CuAAC 和 ROMP

• DOI: 10.1002/macp.202100194
• 发表时间: 2021
• 期刊: Macromolecular Chemistry and Physics
• 影响因子: 2.5
• 作者: A. Saal;C. Friebe;U. S. Schubert
• 通讯作者: U. S. Schubert

Structural Improvement of the Blatter Radical for High-Current Organic Batteries

• DOI: 10.1021/acsaem.2c02559
• 发表时间: 2022-12
• 期刊: ACS Applied Energy Materials
• 影响因子: 6.4
• 作者: Adrian Saal;Lada Elbinger;Kristin Schreyer;Xhesilda Fataj;C. Friebe;U. Schubert