Supramolecular polymerization using two-dimensional π-conjugated chiral monomers has been mainly demonstrated because the supramolecular polymerization can be controlled by stereocommunication through π-π stacking between the two-dimensional chiral monomers. We herein report supramolecular copolymerization utilizing three-dimensional pentahedrons with twisted helical chirality through different combinations of helical-chiral acidic and basic pillar[5]arenes as comonomers. In this case, helical-sense matching is key to facilitating the supramolecular copolymerization.
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