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The growing popularity of quasi-solid-state supercapacitors inevitably leads to the unrestricted consumption of commonly used petroleum-derived polymer electrolytes, causing excessive carbon emissions and resulting in global warming. Also, the porosity and liquid electrolyte uptake of existing polymer membranes are insufficient for well-performed supercapacitors under high current and long cycles. To address these issues, poly(lactic acid) (PLA), a widely applied polymers in biodegradable plastics is employed to fabricate a renewable biocomposite membrane with tunable pores with the help of non-solvent phase inversion method, and a small amount of poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) is introduced as a modifier to interconnect with PLA skeleton for stabilizing the porous structure and optimizing the aperture of the membrane. Owing to easy film-forming and tunable non-solvent ratio, the porous membrane possesses high porosity (ca. 71%), liquid electrolyte uptake (366%), and preferable flexibility endowing the GPE with satisfactory electrochemical stability in coin and flexible supercapacitors after long cycles. This work effectively relieves the environmental stress resulted from undegradable polymers and reveals the promising potential and prospects of the environmentally friendly membrane in the application of wearable devices. [ABSTRACT FROM AUTHOR]

Low energy density hinders the development of supercapacitors in the market of large hybrid power equipment and electric vehicles that demand much higher energy density. Herein, we conduct a facile and environmentally friendly method to modify the electrodes of supercapacitors through coating a dielectric thin film by atomic layer deposition (ALD) technique, which profoundly improves the electrochemical performance of the electrodes. In specific, the gravimetric capacitance of the ALD-Ti modified electrodes is characterized by 35% significant promotion comparing to the commercialized pristine counterparts, and the operational voltage window of the ALD treated electrodes can expand to 3.5 V using organic electrolyte with remarkable capacitance retention (over 83%) even after 20000 cycles. Besides, appropriate models are established to discuss the detailed charge storage mechanism and possible reasons for good stability of modified electrodes under higher operational voltage. Moreover, the excellent rate and cycling performance of ALD modified electrodes in flexible electrochemical double-layer capacitor (EDLCs) at the bending state substantiates the application superiority of ALD modified electrodes in flexible devices. The unusual combination of charge storage mechanisms of dielectric capacitors and EDLCs established in our work represents specific properties in great need for energy storage applications. Atomic Layer Deposition technique is utilized to modify the electrodes in supercapacitors, the modified electrodes can endure the electrochemical window of 3.5 V in organic electrolyte and possesses 35% higher capacitance compared to pristine carbon electrode with longer lifespan. [Display omitted] • The modified electrode increases 35% higher capacitance compared to original one. • The voltage window of treated electrode extends to 3.5 V in organic electrolyte. • The modified flexible devices demonstrate excellent cycling performance. [ABSTRACT FROM AUTHOR]