Thermal aging mechanism of PEDOT:PSS cathodes in stacked aluminum polymer capacitors
摘要
Stacked aluminum polymer capacitors (SAPCs) offer superior volumetric efficiency and exceptionally low equivalent series resistance (ESR), making them ideal for high-power-density electronics. However, their reliability at elevated temperatures remains a critical bottleneck, primarily due to degradation of the PEDOT:PSS cathode. This study systematically investigates the high-temperature degradation mechanisms of SAPCs by directly correlating device-level monitoring with material-level spectroscopic and microstructural characterization. Multi-parameter monitoring under thermal stress identifies ESR as the most sensitive and dominant indicator of device degradation, outpacing changes in capacitance, dissipation factor, and DC leakage current. To elucidate the physical origins of this ESR drift, device-relevant PEDOT:PSS films are thermally aged and evaluated experimentally. The analysis reveals two coupled pathways. First, thermally activated morphological reconstruction occurs through segregation of the insulating PSS phase, which thickens inter-domain barriers and disrupts the conductive network. Second, molecular-level chemical degradation proceeds through progressive dedoping of the PEDOT backbone, driving a transition from highly conductive polaronic states toward neutral states. Based on these results, a thermal degradation model is proposed to link cathode-material evolution to ESR-dominant device aging, providing practical guidance for reliability-oriented design of SAPCs intended for elevated temperature operation.