A flexible supercapacitor (SC) is an attractive energy storage device for powering low-power sensors, since it can be built using only nontoxic and sustainable materials. In this study, the advantages of using biodegradable polylactic acid (PLA) substrate for printed SC are investigated by studying the SC’s cyclic bending reliability, failure mechanism, and the impact of the bending radius. The results confirm that the SCs with laminated PLA with polymer barrier substrate exhibited the highest bending reliability, stability, and capability in preventing liquid electrolyte evaporation among the investigated substrates. Besides, the reliability decreased with the decreasing bending radius only when the strongly impacted areas lie on the electrode, the flaking and cracking of which was found to be the failure mechanisms of the tested SCs, except for the SCs with PLA/Al substrate, which failed due to the Al cracking. This research suggests that using PLA/barrier substrate, developing more robust activated carbon electrodes, developing cellulose paper with more dense fiber structure and smaller porous areas, and controlling the bending radius are crucial to improving the SC’s reliability.
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