Mechanosensitive non-equilibrium supramolecular polymerization in closed chemical systems

Xianhua Lang, Yingjie Huang, Lirong He, Yixi Wang, Udayabhaskararao Thumu, Zonglin Chu, Wilhelm T. S. Huck and Hui Zhao ()
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Xianhua Lang: Sichuan University
Yingjie Huang: Sichuan University
Lirong He: Sichuan University
Yixi Wang: University of Electronic Science and Technology of China
Udayabhaskararao Thumu: University of Electronic Science and Technology of China
Zonglin Chu: Hunan University
Wilhelm T. S. Huck: Radboud University
Hui Zhao: Sichuan University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Chemical fuel-driven supramolecular systems have been developed showing out-of-equilibrium functions such as transient gelation and oscillations. However, these systems suffer from undesired waste accumulation and they function only in open systems. Herein, we report non-equilibrium supramolecular polymerizations in a closed system, which is built by viologens and pyranine in the presence of hydrazine hydrate. On shaking, the viologens are quickly oxidated by air followed by self-assembly of pyranine into micrometer-sized nanotubes. The self-assembled nanotubes disassemble spontaneously over time by the reduced agent, with nitrogen as the only waste product. Our mechanosensitive dissipative system can be extended to fabricate a chiral transient supramolecular helix by introducing chiral-charged small molecules. Moreover, we show that shaking induces transient fluorescence enhancement or quenching depending on substitution of viologens. Ultrasound is introduced as a specific shaking way to generate template-free reproducible patterns. Additionally, the shake-driven transient polymerization of amphiphilic naphthalenetetracarboxylic diimide serves as further evidence of the versatility of our mechanosensitive non-equilibrium system.

Date: 2023
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DOI: 10.1038/s41467-023-38948-x

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