Secondary Nucleation-Triggered Physical Cross-Links and Tunable Stiffness in Seeded Supramolecular Hydrogels

Laishram, R and Sarkar, S and Seth, I and Khatun, N and Aswal, VK and Maitra, U and George, SJ (2022) Secondary Nucleation-Triggered Physical Cross-Links and Tunable Stiffness in Seeded Supramolecular Hydrogels. In: Journal of the American Chemical Society, 144 (25). pp. 11306-11315.

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Abstract

Mechanistic understanding and the control of molecular self-assembly at all hierarchical levels remain grand challenges in supramolecular chemistry. Functional realization of dynamic supramolecular materials especially requires programmed assembly at higher levels of molecular organization. Herein, we report an unprecedented molecular control on the fibrous network topology of supramolecular hydrogels and their resulting macroscopic properties by biasing assembly pathways of higher-order structures. The surface-catalyzed secondary nucleation process, a well-known mechanism in amyloid fibrilization and chiral crystallization of small molecules, is introduced as a non-covalent strategy to induce physical cross-links and bundling of supramolecular fibers, which influences the microstructure of gel networks and subsequent mechanical properties of hydrogels. In addition, seed-induced instantaneous gelation is realized in the kinetically controlled self-assembled system under this study, and more importantly, the extent of secondary nucleation events and network topology is manipulated by the concentration of seeds. © 2022 American Chemical Society.

Item Type:	Journal Article
Publication:	Journal of the American Chemical Society
Publisher:	American Chemical Society
Additional Information:	The copyright for this article belongs to the American Chemical Society.
Keywords:	Gelation; Hydrogels; Nucleation; Stereochemistry; Supramolecular chemistry, Grand Challenge; Hierarchical level; Mechanistics; Molecular self assembly; Network topology; Physical cross-links; Secondary nucleation; Supramolecular hydrogels; Supramolecular materials; Tunable stiffness, Network topology, chemistry; crystallization; hydrogel, Crystallization; Hydrogels
Department/Centre:	Division of Chemical Sciences > Organic Chemistry
Date Deposited:	13 Sep 2022 06:41
Last Modified:	13 Sep 2022 06:41
URI:	https://eprints.iisc.ac.in/id/eprint/76699

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