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Supramolecular copolymerization driven by integrative self-sorting of hydrogen-bonded rosettes.

Aratsu, K; Takeya, R; Pauw, BR; Hollamby, M; Kitamoto, Y; Shimizu, N; Takagi, H; Haruki, R; Adachi, S-I; Yagai, S

Supramolecular copolymerization driven by integrative self-sorting of hydrogen-bonded rosettes. Thumbnail


K Aratsu

R Takeya

BR Pauw

Y Kitamoto

N Shimizu

H Takagi

R Haruki

S-I Adachi

S Yagai


Molecular recognition to preorganize noncovalently polymerizable supramolecular complexes is a characteristic process of natural supramolecular polymers, and such recognition processes allow for dynamic self-alteration, yielding complex polymer systems with extraordinarily high efficiency in their targeted function. We herein show an example of such molecular recognition-controlled kinetic assembly/disassembly processes within artificial supramolecular polymer systems using six-membered hydrogen-bonded supramolecular complexes (rosettes). Electron-rich and poor monomers are prepared that kinetically coassemble through a temperature-controlled protocol into amorphous coaggregates comprising a diverse mixture of rosettes. Over days, the electrostatic interaction between two monomers induces an integrative self-sorting of rosettes. While the electron-rich monomer inherently forms toroidal homopolymers, the additional electrostatic interaction that can also guide rosette association allows helicoidal growth of supramolecular copolymers that are comprised of an alternating array of two monomers. Upon heating, the helicoidal copolymers undergo a catastrophic transition into amorphous coaggregates via entropy-driven randomization of the monomers in the rosette.

Journal Article Type Article
Acceptance Date Mar 9, 2020
Publication Date Apr 1, 2020
Journal Nature Communications
Print ISSN 2041-1723
Peer Reviewed Peer Reviewed
Volume 11
Article Number 1623
Keywords Polymer synthesis; Supramolecular polymers
Publisher URL


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