Precision Design of Sequence‐Defined Polyurethanes: Exploring Controlled Folding Through Computational Design DOI
С.М. Самохвалова, Jean‐François Lutz, Ivan Coluzza

et al.

Macromolecular Chemistry and Physics, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 15, 2024

Abstract This study presents the exploration of sequence‐defined polyurethanes (PUs) as a new class heteropolymers capable precise conformational control. Utilizing molecular dynamics simulations, folding behavior polyurethane chains is investigated varying lengths (11, 20, and 50 monomers) in both vacuum aqueous environments. The simulations reveal that heterogeneous systematically refold to approach designed target structures better than non‐designed or with artificially disrupted hydrogen‐bond networks. subsequent synthesis an optimized 11‐mer sequence (P1) achieved through solid‐phase chemistry, thorough characterization via NMR, MS, SEC confirming accuracy predicted its controlled chain length. Solubility tests showed favorable results across multiple solvents, highlighting versatility polymer. research underscores potential emulate structural functional attributes biological macromolecules, opening pathways for their application catalysis, drug delivery, advanced material design. findings illustrate promising direction development synthetic polymers tailored properties, emphasizing transformative impact control polymer chemistry.

Language: Английский

Sequence of monomers and position of stereocenters matter for thermal properties of stereocontrolled oligourethanes DOI
Weronika Forysiak, Agnieszka Lizak, Róża Szweda

et al.

ChemPhysChem, Journal Year: 2024, Volume and Issue: 25(17)

Published: May 16, 2024

Polyurethanes are commodity materials used for multiple applications. In recent years, a new category of polyurethane material has emerged, characterized by the lack polymer molar mass dispersity, control monomer arrangement in chain, and even full stereocontrol. Various multistep synthesis strategies have been developed to fabricate sequence-defined polyurethanes. However, synthesizing stereocontrolled polyurethanes with controlled sequence is still challenge. structural precision, as represented biopolymers, i. e. proteins or nucleic acids, opened application directions these groups materials. It shown that can be biomimetics, information carriers, molecular tags, strictly properties. Precise macromolecules allows us fine-tune properties polymers specific needs. Therefore, it essential collect on sequence-structure relationship polymers. our work, we present synthetic pathways make stereo-defined oligourethanes. We demonstrate details, e., sequences position stereocenter, tremendous effect thermal model show introduction chirality constitutional isomerization program characteristics polymers, which key features

Language: Английский

Citations

1

Sequence-defined structural transitions by calcium-responsive proteins DOI Creative Commons
Marina P. Chang, Winnie Huang,

Gatha Shambharkar

et al.

Published: Aug. 20, 2024

Biopolymer sequences dictate their functions, and protein-based polymers are a promising platform to establish sequence–function relationships for novel biopolymers. To efficiently explore vast sequence spaces of natural proteins, repetition is common strategy tune amplify specific functions. This applied repeats-in-toxin (RTX) proteins with calcium-responsive folding behavior, which stems from tandem repeats the nonapeptide GGXGXDXUX in X can be any amino acid U hydrophobic acid. determine functional range this nonapeptide, we modified naturally occurring RTX protein that forms β-roll structures presence calcium. Sequence modifications focused on calcium-binding turns within repetitive region, including either global substitution nonconserved residues or complete replacement consensus GGAGXDTLY. Some disrupted typical transition intrinsically disordered random coils folded β rolls, despite conservation underlying sequence. Proteins enriched smaller, acids adopted secondary absence calcium underwent structural rearrangement calcium-rich environments. In contrast, bulkier, hydrophilic maintained intrinsic disorder These results indicate significant role folding, thereby revealing leverage design tunable,

Language: Английский

Citations

1

Sequence-defined structural transitions by calcium-responsive proteins DOI
Marina P. Chang, Winnie Huang, Gatha M. Shambharkar

et al.

Polymer Chemistry, Journal Year: 2024, Volume and Issue: 15(47), P. 4864 - 4874

Published: Jan. 1, 2024

Recombinant protein engineering accelerated the synthesis of sequence-defined, calcium-responsive biopolymers. A mutation panel repeats-in-toxin (RTX) proteins revealed sequence-dependent disorder, calcium sensitivity, and structural transitions.

Language: Английский

Citations

1

Precision Design of Sequence‐Defined Polyurethanes: Exploring Controlled Folding Through Computational Design DOI
С.М. Самохвалова, Jean‐François Lutz, Ivan Coluzza

et al.

Macromolecular Chemistry and Physics, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 15, 2024

Abstract This study presents the exploration of sequence‐defined polyurethanes (PUs) as a new class heteropolymers capable precise conformational control. Utilizing molecular dynamics simulations, folding behavior polyurethane chains is investigated varying lengths (11, 20, and 50 monomers) in both vacuum aqueous environments. The simulations reveal that heterogeneous systematically refold to approach designed target structures better than non‐designed or with artificially disrupted hydrogen‐bond networks. subsequent synthesis an optimized 11‐mer sequence (P1) achieved through solid‐phase chemistry, thorough characterization via NMR, MS, SEC confirming accuracy predicted its controlled chain length. Solubility tests showed favorable results across multiple solvents, highlighting versatility polymer. research underscores potential emulate structural functional attributes biological macromolecules, opening pathways for their application catalysis, drug delivery, advanced material design. findings illustrate promising direction development synthetic polymers tailored properties, emphasizing transformative impact control polymer chemistry.

Language: Английский

Citations

0