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

Keisuke Aratsu, Rika Takeya, Brian R. Pauw (), Martin J. Hollamby (), Yuichi Kitamoto, Nobutaka Shimizu, Hideaki Takagi, Rie Haruki, Shin-ichi Adachi and Shiki Yagai ()
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Keisuke Aratsu: Chiba University
Rika Takeya: Chiba University
Brian R. Pauw: BAM Federal Institute for Materials Research and Testing Unter den Eichen 87
Martin J. Hollamby: Keele University
Yuichi Kitamoto: Chiba University
Nobutaka Shimizu: High Energy Accelerator Research Organization
Hideaki Takagi: High Energy Accelerator Research Organization
Rie Haruki: High Energy Accelerator Research Organization
Shin-ichi Adachi: High Energy Accelerator Research Organization
Shiki Yagai: Chiba University

Nature Communications, 2020, vol. 11, issue 1, 1-12

Abstract: Abstract 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.

Date: 2020
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DOI: 10.1038/s41467-020-15422-6

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