Synthesis and self-assembly of bottlebrush block copolymer electrolytes for solid-state supercapacitors

All-solid-state supercapacitors have attracted increasing attention in recent decades owing to rapid advancements in safe, flexible, and wearable energy storage devices. This study demonstrates a bottlebrush block copolymer electrolyte consisting of poly(styrene-b-butadiene-b-styrene)-g-poly(ethylene glycol) behenyl ether methacrylate (SBS-g-PEGBEM) (simply SgP) for all-solid-state supercapacitors. Due to the adhesive nature and robust mechanical properties of SgP film, devices can be manufactured without the need for separators or packaging. The nonpolar SBS domains serve as scaffolds within the polymer matrix, while the polar PEGBEM domains offer interactive sites for polar ionic liquids (ILs). The synergy between precisely defined nanostructures and the subsequent well-dissociated ions enhances efficient ion transport through the ionic channels. As a result, the supercapacitor with SgP/IL electrolyte exhibits remarkable electrochemical performance. This includes a wide potential window of 2.4 V, an ionic conductivity of 2.4 mS cm−1, and maximum energy density and power density of 28.1 Wh kg−1 and 3080 W kg−1, respectively. The supercapacitor also demonstrates high cycle stability with 87.7 % capacitance retention after 5,000 cycles. The positive impact of the PEGBEM side chains is investigated via molecular dynamics simulations. Thus, this study presents a novel strategy for solid-state electrolytes, offering potential advancements in next-generation energy storage devices.