Hard–soft–hard triblock copolymers based on poly­(ethylene oxide) (PEO), poly­(2-naphthyl glycidyl ether)-block-poly­[2-(2-(2-methoxy­ethoxy)­ethoxy)­ethyl glycidyl ether]-block-poly­(2-naphthyl glycidyl ether)­s (PNG-PTG-PNGs), were synthesized by sequential ring-opening polymerization of 2-(2-(2-methoxy­ethoxy)­ethoxy)­ethyl glycidyl ether and 2-naphthyl glycidyl ether using a bidirectional initiator catalyzed by a phosphazene base. Four PNG-PTG-PNGs had different block compositions (f wt,PNG = 9.2–28.6 wt %), controlled molecular weights (M n = 23.9–30.9 kDa), and narrow dispersities (Đ = 1.11–1.14). Most of the PNG-PTG-PNG electrolytes had much higher Li+ conductivities than that of a PEO electrolyte (6.54 × 10–7 S cm–1) at room temperature. Eespecially, the Li+ conductivity of PNG18-PTG107-PNG18 electrolyte (9.5 × 10–5 S cm–1 for f wt,PNG = 28.6 wt %) was comparable to one of a PTG electrolyte (1.11 × 10–4 S cm–1). The Li+ conductivities of PNG-PTG-PNG electrolytes were closely correlated to efficient Li+ transport channels formed by the microphase separation into soft PTG and hard PNG domains.

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Considerable research approaches have focused on improving the crystallinity of conducting polymers to enhance the electrical conductivity. However, it is difficult to control the arrangement of polymer chains without the use of expensive and complex methods because of the intrinsic morphology of polymers. Herein, we report a one-step in situ process to produce controlled molecular-scale ordered polyaniline (PANI) films by coordination crosslinking with Zn ions using solvent-vapor thermal annealing (SVTA). The resulting PANI film crosslinked by Zn coordination has a face-centered cubic structure at the molecular scale, which was confirmed by high-voltage electron microscopy. The in situ coordination crosslinking produced a new class of molecular ordering in the PANI films and drastically enhanced their conductivity, showing their potential for use in various electronic and energy devices.