The
shapeshifting behavior for synthetic matters was found at either
the molecular or supramolecular level, but the connection between
shapeshifting at the two hierarchical levels remains missing. In this
study, an 8-arm star giant molecule, NPOSS, was synthesized
to connect the molecular and supramolecular shapeshifting. Controlling
the conditions of bulk self-assembly allowed us to bring NPOSS into three different Ostwald’s stages of nucleation. The
high conformational flexibility of NPOSS facilitates
molecular shapeshifting and allows NPOSS to take the
discotic, rod-like and star-like geometries in different Ostwald’s
stages. Simultaneous changes in the supramolecular scaffolds were
observed as the discotic, rod-like and star-like NPOSS molecules self-assembled into the supramolecular scaffolds of 1D
columns, 2D lamellae, and 3D networks, respectively. These changes
in the hierarchical structures also affect the CO2 affinity
of NPOSS. Therefore, the connection between the molecular/supramolecular
shapeshifting and the structure-driven property changes of NPOSS were established by taking advantage of the high conformational
freedom of the 8-arm star giant molecule and its diverse self-assembly
pathways leading to the different Ostwald’s stages.
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