Organomediated polymerization

Honda, Satoshi; Odelius, Karin; Sardon, Haritz

doi:10.1038/s42004-024-01134-1

Commun Chem

2024

DOI: 10.1038/s42004-024-01134-1

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Organomediated polymerization

Satoshi Honda,

Karin Odelius,

Haritz Sardon

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2024

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High Molecular Weight Protein-Like Semiflexible Chains via Bioorthogonal Polymerization of Coiled-Coil Peptides

Gao,

Zhang,

Langenstein

et al. 2024

Macromolecules

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Peptides capable of forming homotetrameric coiledcoil bundles are utilized as monomeric building blocks ("bundlemers") to synthesize protein-like hybrid polymers consisting of covalently linked coiled-coil microdomains with regularly spaced ethylene glycol repeats via step-growth polymerization employing the highly efficient, bioorthogonal tetrazine (Tz) ligation with trans-cyclooctene (TCO). Polymerization of Tz and TCO-functionalized peptides in aqueous media under strict stoichiometry at Tz or TCO concentrations of 0.1 to 4.5 mM leads to the establishment of exceptionally long, semiflexible polymer chains with a Kuhn length of 6−7 nm and an apparent molecular weight up to 3 MDa. Bioorthogonal polymerization at bundlemer concentrations above 5 mM gives rise to physical gels through interchain entanglements. Hydrogels prepared at 10 mM exhibit an average elastic modulus of 400 Pa and a strain to failure of 300%. Copolymerization of coiled-coil peptides with distinct composition and thermal stability results in hydrogels that are thermally tunable. A solid-to-fluid transition occurs when one of the coiled-coil repeats melts. Upon cooling, solid-like properties are partially recovered through the intermolecular association of the helical peptides. Overall, tetrazine ligation has enabled the covalent polymerization of self-assembled coiled-coil motifs for the establishment of protein-like linear polymers with unprecedented molecular weight.

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High Molecular Weight Protein-Like Semiflexible Chains via Bioorthogonal Polymerization of Coiled-Coil Peptides

Gao,

Zhang,

Langenstein

et al. 2024

Macromolecules

View full text Add to dashboard Cite

show abstract

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Organomediated polymerization

Cited by 1 publication

References 18 publications

High Molecular Weight Protein-Like Semiflexible Chains via Bioorthogonal Polymerization of Coiled-Coil Peptides

High Molecular Weight Protein-Like Semiflexible Chains via Bioorthogonal Polymerization of Coiled-Coil Peptides

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