The number of portable devices produced worldwide is strongly increasing, which results in an increasing need for energy storage devices. These devices are typically fabricated with scarce and toxic materials. Consequently, there is a current trend towards the substitution of these materials by biopolymers, although they are still often mixed with toxic substances to improve specific performance aspects. To address this issue, this work presents a self-standing non-toxic and potentially biodegradable polymer electrolyte membrane for electrochemical energy storage applications consisting of an abundant biopolymer, iota-carrageenan, and Deep Eutectic Solvent (DES).11List of abbreviations: DES: Deep eutectic solvent [EMIM][SCN]: 1-Ethyl-3-methyl-imidazolium thiocyanate CV: Cyclic voltammetry FTIR: Fourier transformed infrared spectroscopy EIS: Electrochemical impedance spectroscopy CPE: Constant phase element. Ionic conductivities as high as 2 mS/cm were achieved for a proportion of carrageenan and DES of 25:75. Aqueous electrically conductive inks containing carbon black and active carbon were also developed using the same polymeric matrix. The inks were successfully printed (stencil method) on different substrates and electrically characterized, achieving sheet resistances as low as 38 Ω/sq. Supercapacitors were then fabricated by printing the electrically conductive ink on both sides of the self-standing membrane, demonstrating the versatility of iota-carrageenan biopolymer in the development of sustainable energy storage devices. The measured capacitance of the supercapacitors was 3.3 mF/cm2 in cyclic voltammetry characterization and 2.7 mF/cm2 when charging-discharging at 0.05 mA/cm2. The supercapacitors were found to be stable in cyclability studies, showing a capacity retention of 99 % after 5000 charge–discharge cycles.
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