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• Rubbery SBS-g-POEM amphiphilic copolymer showed excellent compatibility with ZIF-8. • MMMs with SBS showed a continuous decrease in selectivity. • MMMs with SBS-g-POEM achieved simultaneous improvement in permeability and selectivity. • MMMs exhibited good mechanical strength and excellent thermal stability up to 300 °C. We report the development and assessment of mixed-matrix membranes (MMMs) that showed simultaneous improvement in CO 2 permeability and CO 2 /N 2 selectivity based on precise interface and interaction control. Specifically, MMMs were prepared using solution-synthesized ZIF-8 nanoparticles dispersed in a rubbery amphiphilic copolymer matrix, namely, poly(styrene- b -butadiene- b -styrene)- g -poly(oxyethylene methacrylate) (SBS-g-POEM) synthesized by free-radical polymerization. Excellent interface contact and compatibility between the ZIF-8 nanoparticles and SBS-g-POEM matrix were confirmed. The results showed that the polymer matrix did not damage the nanostructure of the ZIF-8, and the POEM chains grafted from the SBS backbones enhanced the compatibility with the ZIF-8. While the MMM based on a neat SBS matrix showed a continuous decrease in selectivity, the MMM based on SBS-g-POEM achieved a simultaneous improvement in permeability (from 261.7 to 522.3 Barrer) and CO 2 /N 2 selectivity (from 18.6 to 20.8), indicating the importance of the matrix in tuning the interface and interaction of MMMs. The obtained CO 2 /N 2 separation performance is close to the upper bound and one of the highest values for ZIF-8-based MMMs. Furthermore, the MMMs exhibited good mechanical strength (8.5 MPa tensile stress and 940% strain) and excellent thermal stability at least up to 300 °C. [ABSTRACT FROM AUTHOR]

• PEGBEM-g-PAEMA graft copolymer is synthesized via free-radical polymerization. • The electrolyte maintained its flexible solid film state for EMIMBF 4 content up to 200%. • The solid capacitors exhibited good bending performance without specific encapsulation. • The capacitors with PEGBEM-g-PAEMA exhibited better performance compared with other polymer/EMIMBF 4 cells. We report a solid electrolyte comprising poly(ethylene glycol) behenyl ether methacrylate-g-poly((2-acetoacetoxy)ethyl methacrylate) (PEGBEM-g-PAEMA) graft copolymer for application to solid-state bendable supercapacitors. The graft copolymer was synthesized via free-radical polymerization, and the electrolytes were fabricated by adding 1-ethyl-3-methylimidazolium tetrafluoroborate (EMIMBF 4). Fourier-transform infrared spectroscopy, differential scanning calorimetry, thermogravimetric analysis, X-ray diffraction, small-angle X-ray scattering, and transmission electron microscopy were employed to investigate the chemical, structural, thermal, and morphological properties of the fabricated electrolytes and the compatibility of the two components. The graft copolymer interacted with EMIMBF 4 (the two materials were compatible with each other), and the intruded ionic liquid was well-dispersed through the entire region of the polymer matrix. The fabricated electrolyte maintained its flexible solid film state for EMIMBF 4 content up to 200% without leakage problems. The capacitors were manufactured with porous carbon electrodes and a PEGBEM-g-PAEMA/EMIMBF 4 electrolyte. The capacitors exhibited a capacitance of 55.5F/g, a power density of 900 W/kg, and an energy density of 25 Wh/kg at 1.0 A/g. The capacitors were measured at various bending angles and exhibited good performance without specific encapsulation. According to the results, the newly synthesized PEGBEM-g-PAEMA graft copolymer is a good candidate for a polymer matrix for electrolytes in all-solid-state bendable/flexible supercapacitors. [ABSTRACT FROM AUTHOR]