Living supramolecular polymerization of fluorinated cyclohexanes

Shyshov, Oleksandr; Haridas, Shyamkumar Vadakket; Pesce, Luca; Qi, Haoyuan; Gardin, Andrea; Bochicchio, Davide; Kaiser, Ute; Pavan, Giovanni M.; Delius, Max von

doi:10.1038/s41467-021-23370-y

Cited by 51 publications

(55 citation statements)

References 84 publications

(90 reference statements)

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“…Because PCs include the varied influences of original features, 93 differences between the clusters can be traced back to changes in these features as a function of amphiphilic architecture or temperature. This information is captured in loading plots ( Figure 5 c), which elucidates the contribution of features to each PC on a normalized scale, −1 to 1.…”

Section: Resultsmentioning

confidence: 99%

Adaptive Recombinant Nanoworms from Genetically Encodable Star Amphiphiles

Hossain

Lynch

et al. 2021

Biomacromolecules

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Recombinant nanoworms are promising candidates for materials and biomedical applications ranging from the templated synthesis of nanomaterials to multivalent display of bioactive peptides and targeted delivery of theranostic agents. However, molecular design principles to synthesize these assemblies (which are thermodynamically favorable only in a narrow region of the phase diagram) remain unclear. To advance the identification of design principles for the programmable assembly of proteins into well-defined nanoworms and to broaden their stability regimes, we were inspired by the ability of topologically engineered synthetic macromolecules to acess rare mesophases. To test this design principle in biomacromolecular assemblies, we used post-translational modifications (PTMs) to generate lipidated proteins with precise topological and compositional asymmetry. Using an integrated experimental and computational approach, we show that the material properties (thermoresponse and nanoscale assembly) of these hybrid amphiphiles are modulated by their amphiphilic architecture. Importantly, we demonstrate that the judicious choice of amphiphilic architecture can be used to program the assembly of proteins into adaptive nanoworms, which undergo a morphological transition (sphere-to-nanoworms) in response to temperature stimuli.

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Section: Resultsmentioning

confidence: 99%

Adaptive Recombinant Nanoworms from Genetically Encodable Star Amphiphiles

Hossain

Lynch

et al. 2021

Biomacromolecules

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“…The ability to continuously incorporate new monomers from solution into a nanostructure imbues these types of supramolecular polymers with a 'living' characteristic 14,15 analogous to traditional living covalent polymerizations. A 'living' supramolecular polymer has chain ends (1D) or edges (2D) that remain active even after all of the monomers have been consumed in the reaction mixture, thereby allowing the supramolecular polymer to continue growing upon addition of more monomers to the reaction mixture.…”

Section: Nucleation and Growth Pathwaysmentioning

confidence: 99%

Designing supramolecular polymers with nucleation and growth processes

Bruckner

Stupp

2022

Polymer International

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The self‐assembly of small molecules into supramolecular polymers can be analogous to the formation of classical solid‐state crystals depending on the mechanism of polymerization. Taking inspiration from the field of materials science, complex supramolecular polymer nanostructures can be formed by carefully controlling nucleation and growth processes. Exploration of the energy landscapes in supramolecular polymers can also lead to the discovery of polymorphs where a single monomer can self‐assemble into different supramolecular polymers with distinct molecular packing arrangements. This mini‐review focuses on recent developments where the manipulation of nucleation and growth processes were used to develop novel supramolecular copolymers and explore polymorphism in supramolecular materials, highlighting examples of such systems composed of small organic molecules and peptides. © 2022 The Authors. Polymer International published by John Wiley & Sons Ltd on behalf of Society of Industrial Chemistry.

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“…3G and H ). 58–64 Seeding effects originate from a template-accelerated growth that occurs on small aggregate fragments – usually obtained after fragmentation (by sonication) of nano-assemblies ( e.g. fibers and micelles) 65–67 – which trigger supramolecular living polymerization by overriding the energy barriers ( Fig.…”

Section: Supramolecular Polymers Made Of Aromatic-peptide Conjugatesmentioning

confidence: 99%

“…However, it is the recent discovery of living supramolecular polymerization that is really facilitating the preparation of supramolecular block copolymers, and several examples based on different molecular designs have been recently reported by the George, 223–226 Würthner, 227 and von Delius 58 groups – all using two-component seeded living polymerization yielding very long fibres with a very limited length dispersity.…”

Section: Recent Developmentsmentioning

confidence: 99%