Designing polymer-based organic thin-film batteries towards IoT applications.

物联网(IoT)家电要求电池不仅耐用、环保、节约和廉价，而且还需要能够在数据传输过程中提供间歇性高电流突发。有机基电池有可能满足所有这些要求。该项目的目标包括优化使用锂金属阳极运行的多层聚合物有机电池，使其朝着更高的功率密度发展，以适应物联网应用所需的短充放电脉冲。为了了解潜在的电子和离子传输机制，将采用一种整体的方法，包括合成有机阴极材料和特定匹配的聚合物电解质，深入的电化学表征，多峰电子顺磁共振(EPR)分析和计算模拟。虽然将利用广泛的电和物理化学测量来评估材料和电池系统的可实现性能，特别是在高C率下的充放电和长期循环稳定性方面，但定制的EPR技术，包括在OPANDO光谱-电化学测量中，将发挥核心作用，以揭示自由基物种的分布及其在阴极复合材料中作为电荷状态的函数的相互作用。这样，一方面将建立细胞容量与健康状态之间的关系，另一方面将建立自由基密度和电子迁移率之间的关系，这将被用来进一步优化实际的细胞化学。为了在分子水平上获得更多的洞察力，将应用分子动力学(MD)模拟来推导阴极复合材料内和阴极-电解液界面上的离子扩散系数和电导率。这些工作将有助于解释EPR、PFG-核磁共振和阻抗数据，以及设计具有所需界面性质的新型阴极和电解液材料，从而促进电池内电极之间的电荷转移。从分子动力学模拟中采集的分子结构将经过量子化学计算，以获得与电子传输相关的关键参数以及EPR观测值。结合电化学数据，这些努力将被用来在实验上增强阴极中的电子传输。所获得的知识将被用于开发全聚合ORB的原型，从而验证细胞设计的协同方法并使物联网应用成为可能。

Internet of things (IoT) appliances require batteries that are not only long lasting, environmentally friendly, save and cheap, but they also need to be capable of providing intermittent high current bursts during data transmission. Organic radical batteries potentially meet all these requirements. The goals of this project include optimization of multilayered polymeric organic batteries operating with lithium metal anodes towards higher power densities to accommodate short charge and discharge pulses required for IoT applications. To understand the underlying electron and ion transport mechanisms, a holistic approach comprising synthesis of organic cathode materials and specifically matched polymer electrolytes, in-depth electrochemical characterization, multimodal electron paramagnetic resonance (EPR) analyses and computational modeling will be employed. While a wide range of electro- and physicochemical measurements will be utilized to assess achievable performance of both materials and cell systems, especially with respect to charge/discharge at high C-rates and long-term cycling stability, tailored EPR techniques, including in operando spectro-electrochemical measurements, will play a central role to unravel distributions of radical species and their interaction within the cathode composite as a function of the state of charge. In this way, the relation between cell capacity and state of health on the one hand, and the radical density and electron mobility on the other hand will be established, which will be exploited to further optimize actual cell chemistries. To gain additional insight at the molecular level, molecular dynamics (MD) simulations will be applied to derive ionic diffusivities and conductivities both within the cathode composite and at cathode|electrolyte interfaces. These efforts will be helpful to interpret EPR, PFG-NMR and impedance data, as well as to design novel cathode and electrolyte materials with desired interfacial properties, thereby boosting charge transfer across electrodes within the cells. Molecular structures sampled from MD simulations will be subjected to quantum chemical calculations to obtain key parameters relevant for electron transport as well as EPR observables. Combined with the electrochemical data, these efforts will be utilized to enhance electronic transport in the cathodes experimentally. The gained knowledge will be exploited to develop a prototype of an all-polymeric ORB, thereby validating the synergistic approach for the design of cells and enabling IoT applications.