A facile oxygen (O2) atmospheric plasma treatment is applied to a polyvinyl alcohol (PVA) matrix to enhance its wettability and hydrophilicity. The optimal plasma treatment conditions are determined by varying the applied plasma power and plasma treatment time. A PVA matrix treated with a plasma power of 120 W for 5 s shows the most hydrophilicity owing to successful formation of carbonyl (–CO, >C=O) functional groups without any structural degradation. The plasma-treated PVA matrix is used as the gel-polymer electrolyte of a solid-state supercapacitor (SSC) by immersing solid matrix into various liquid electrolytes, such as sodium sulfate (Na2SO4), sulfuric acid (H2SO4), and potassium hydroxide (KOH). Compared with the pristine PVA-based device, PVA-120W5/Na2SO4-, PVA-120W5/H2SO4-, and PVA-120W5/KOH-based SSCs show 2.03, 2.05, and 2.14 times higher specific capacitances, respectively. The plasma-treated PVA matrix shows increased specific capacitance owing to the increased wettability, which in turn increases the ion transportation and reduces the electrical resistance. This study successfully demonstrates that the electrochemical performance of a SSC can be readily enhanced through plasma treatment for a short time (≤5 s).
