Characterization of the Interfaces in LiFePO4/PEO-LiTFSI Composite Cathodes and to the Adjacent Layers

Interface resistances between the different components of battery cells limit their fast charge and discharge capability which is required for different applications such as electromobility. To decrease interface resistances, it is necessary to understand which individual interface they arise at and how they can be controlled. Electrochemical impedance spectroscopy is a well-established technique for the distinction of different contributions to the internal cell resistance and allows the characterization of interface resistances. Especially the use of suitable cell setups allows one to attribute the measured resistances to specific interfaces. In this contribution, we investigate the impedance of dry polymer full cells containing a lithium iron phosphate/ poly(ethylene oxide)-lithium bis(trifluoromethanesulfonyl)imide composite cathode, a solid polymer electrolyte separator and a lithium-metal anode. Based on the results on different cell setups, we are able to reliably determine the planar resistances between the components as well as the charge transfer resistance inside the composite cathode. For unoptimized systems, we find high planar resistances, which can be significantly reduced by coating and processing strategies. For the charge transfer resistance, we find a dependence on the SOC as well as on the charging direction. Possible mechanisms for the evolution of interface resistances are discussed also based on chemical analysis performed by photoelectron spectroscopy (XPS)