Isotactic polyacrylonitrile (iso-PAN) is synthesized via template polymerization using the two-dimensional layered space of a CoCl2 crystal as a template. Isotacticity of polyacrylonitrile reaches a meso/meso triad = 93% (mm = 0.93), which indicates a superior packing of polymer chains, leading to a high breakdown strength. Tacticity enhancement is correlated with the interatomic (metal-metal) distance of template-layered crystals. Due to a large dipole moment (4.3 D) of nitrile group and a high stereoregularity, iso-PAN demonstrates a high discharge energy density of 6.7 J/cm3 at 660 MV/m, nearly six times that of atactic polyacrylonitrile (ata-PAN) and biaxially oriented polypropylene (BOPP), a commercially available dielectric polymer film. Moreover, it exhibits a charge-discharge efficiency of ca. 90% in a wide applied electric field range, which is higher than the efficiencies of ata-PAN and BOPP. These results suggest that iso-PAN, exhibiting a large dipole moment and high stereoregularity, is a promising candidate for high energy density and low loss capacitor dielectrics.
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