Triblock copolymers such as styrene-b-(ethylene-co-butylene)-b-styrene (SEBS) have been widely used as an anion exchange membrane for fuel cells due to their phase separation properties. However, modifying the polymer architecture for optimized membrane properties is still challenging. This research develops a strategy to control the membrane morphology based on quaternized SEBS (SEBS-Q) by dual-tapering the interfacial block sequences. The structural and transport properties of SEBS-Q with various tapering styles at different hydration levels are systematically investigated by coarse-grained molecular simulations. The results show that the introduction of the tapered regions induces the formation of a bicontinuous water domain and promotes the diffusivity of the mobile components. The interplay between the solvation of the quaternary groups and the tapered fraction determines the conformation of polymer chains among the hydrophobic–hydrophilic subdomains. The strategy presented here provides a new path to fabricating fuel cell membranes with controlled microstructures.
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