Supramolecular Copolymerization as a Strategy to Control the Stability of Self‐Assembled Nanofibers

Thota, Bala N. S.; Lou, Xianwen; Bochicchio, Davide; Paffen, Tim F. E.; Lafleur, René P. M.; Dongen, Joost L. J. van; Ehrmann, Svenja; Haag, Rainer; Pavan, Giovanni M.; Palmans, Anja R. A.; Meijer, E. W.

doi:10.1002/ange.201802238

Cited by 13 publications

(3 citation statements)

References 34 publications

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“…According to the "majority rules" reported for previous supramolecular systems, [18] it seems that the supramolecular polymer or network in this two-component hydrogel system is not formed by the random coassembly of LPF and LPFEG. [16,19] Instead, it appears to be constructed by independent self-association of LPF and LPFEG separately, namely, self-sorting of the chiral assemblies. [7b, 15c] To prove that self-sorting occurs in this two-component hydrogel system, we conducted some control experiments.…”

Section: Angewandte Chemiementioning

confidence: 99%

Self‐Sorting Double‐Network Hydrogels with Tunable Supramolecular Handedness and Mechanical Properties

et al. 2019

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Section: Angewandte Chemiementioning

confidence: 99%

Self‐Sorting Double‐Network Hydrogels with Tunable Supramolecular Handedness and Mechanical Properties

et al. 2019

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“…However, the interesting issue about this bonding energy spectrum is the fact that supramolecular polymers in which mers are bonded non‐covalently can in principle not only populate the low bonding energy part of the spectrum but also overlap over the entire spectrum depending on the molecular complexity of mers . The monomers of supramolecular polymers investigated so far span a broad range, starting with the simple ones developed initially in which several hydrogen bonds among mers dominate formation of the supramolecular polymer and others where multiple interactions control formation of the polymer . The multiple interactions may involve hydrogen bonding, hydrophobic collapse, π‐orbital overlaps, electrostatics, sterics, metal‐ligand contacts, among other interactions.…”

Section: Introductionmentioning

confidence: 99%

Supramolecular and Hybrid Bonding Polymers

Stupp

Clemons²,

Carrow³

et al. 2020

Israel Journal of Chemistry

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Staudinger established a century ago the existence of covalent macromolecules, work that led to the development of transformative materials of great benefit to society and a “quantum leap” in our understanding of biological systems. Over the past few decades the concept of supramolecular polymers has emerged–chemical systems in which structural units bond strongly to each other non‐covalently. These dynamic systems actually exist in the natural world and can create soft materials with structures, properties, and functions beyond the ones we know in Staudinger polymers. We reflect here on the potential of novel systems in which covalent and supramolecular polymers are chemically integrated and describe them as hybrid bonding polymers. This paper describes the concept with recent examples from the Stupp laboratory, and discusses their potential functions as robotic materials that mimic living matter and structures that offer new ideas on how to recycle and reuse soft materials.

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“…[8][9][10] However, recent reports have shown that the properties of coassembled supramolecular materials can be significantly different than those of the separate components. 11 In this regard, it is crucial to get a comprehensive understanding to which extent the supramolecular interactions in multicomponent systems can direct the properties of soft materials.…”

Section: Introductionmentioning

confidence: 99%

A DNA-Small Molecule Conjugate Modulates the Complexity of Multicomponent Supramolecular Polymerization in Biorelevant Environments

Vybornyi¹,

Wijnands²,

Jeon³

et al. 2020

Preprint

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Aqueous multicomponent supramolecular systems hold great promise for designing synthetic biomaterials with tailored properties. Inspired by this notion, we explore the consequences of modulating the assembly behaviour of supramolecular polymers based on benzene-1,3,5-trixaboxamide (BTA) derivatives by the corresponding BTA-DNA conjugate. Our data demonstrate the divergence of the assembly mechanisms upon shifting from pure water to buffered solutions (pH=7) upon introducing the DNA conjugate. To follow the morphologic transitions, we developed a correlative spectroscopic-microscopic method suitable for the analyses of thermally controlled supramolecular copolymerization in aqueous systems. Using this approach, the structural origins of the cooperative transitions in water-soluble BTA systems were confirmed for the first time. Thus, at the macroscale, the elongation into micrometer-long supramolecular fibers occurs from globular aggregates, which exist at elevated temperatures. The acquired experimental data support the assumption expressed in the previous computational reports that nanoscale BTA ordering within the globules precedes the elongation phase. Furthermore, depending on the content of the DNA modulator, the globules derive two forms of supramolecular fibers, type I and type II, respectively. The latter type is stable within a short temperature window, transforming into the former one upon further cooling. Finally, the supramolecular copolymers were transformed in functional hydrogels via a DNA crosslinking strategy. Physical and mechanical properties of the hydrogels were assessed by microrheology.

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Supramolecular Copolymerization as a Strategy to Control the Stability of Self‐Assembled Nanofibers

Cited by 13 publications

References 34 publications

Self‐Sorting Double‐Network Hydrogels with Tunable Supramolecular Handedness and Mechanical Properties

Self‐Sorting Double‐Network Hydrogels with Tunable Supramolecular Handedness and Mechanical Properties

Supramolecular and Hybrid Bonding Polymers

A DNA-Small Molecule Conjugate Modulates the Complexity of Multicomponent Supramolecular Polymerization in Biorelevant Environments

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