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

物联网（IoT）设备不仅需要电池持久，环保，节省和便宜，而且还需要能够在数据传输期间提供间歇性高电流突发。有机自由基电池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的多层聚合物有机电池，以实现更高的功率密度，以适应物联网应用所需的短充放电脉冲。为了理解潜在的电子和离子传输机制，将采用整体方法，包括有机阴极材料和特定匹配的聚合物电解质的合成，深入的电化学表征，多峰电子顺磁共振（EPR）分析和计算建模。虽然广泛的电和物理化学测量将用于评估材料和电池系统的可实现性能，特别是在高C倍率下的充电/放电和长期循环稳定性方面，但定制的EPR技术，包括操作光谱电化学测量，将在阐明阴极复合材料内自由基物质的分布及其相互作用作为荷电状态的函数方面发挥核心作用。通过这种方式，一方面将建立电池容量和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，这将用于进一步优化实际的电池化学。为了在分子水平上获得更多的了解，将应用分子动力学（MD）模拟来推导阴极复合材料内和阴极处的离子扩散率和电导率|电解质界面这些努力将有助于解释EPR，PFG-NMR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质材料，从而促进电池内电极之间的电荷转移。 从MD模拟中取样的分子结构将进行量子化学计算，以获得与电子输运以及EPR观测值相关的关键参数。结合电化学数据，这些努力将被用来提高电子传输的阴极实验。所获得的知识将用于开发全聚合物ORB的原型，从而验证电池设计的协同方法并实现物联网应用。

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.