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  1. The biological significance of self-assembled protein filament networks and their unique mechanical properties have sparked interest in the development of synthetic filament networks that mimic these attributes. Building on the recent advancement of autoaccelerated ring-opening polymerization of amino acid N-carboxyanhydrides (NCAs), this study strategically explores a series of random copolymers comprising multiple amino acids, aiming to elucidate the core principles governing gelation pathways of these purpose-designed copolypeptides. Utilizing glutamate (Glu) as the primary component of copolypeptides, two targeted pathways were pursued: first, achieving a fast fibrillation rate with lower interaction potential using serine (Ser) as a comonomer, facilitating the creation of homogeneous fibril networks; and second, creating more rigid networks of fibril clusters by incorporating alanine (Ala) and valine (Val) as comonomers. The selection of amino acids played a pivotal role in steering both the morphology of fibril superstructures and their assembly kinetics, subsequently determining their potential to form sample-spanning networks. Importantly, the viscoelastic properties of the resulting supramolecular hydrogels can be tailored according to the specific copolypeptide composition through modulations in filament densities and lengths. The findings enhance our understanding of directed self-assembly in high molecular weight synthetic copolypeptides, offering valuable insights for the development of synthetic fibrous networks and biomimetic supramolecular materials with custom-designed properties. 
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    Free, publicly-accessible full text available March 6, 2025
  2. Abstract

    Inspired by protein polymerizations, much progress has been made in making “polymer‐like” supramolecular structures from small synthetic subunits through non‐covalent bonds. A few regulation mechanisms have also been explored in synthetic platforms to create supramolecular polymers and materials with dynamic properties. Herein, a type of reactive regulator that facilitates the dimerization of the monomer precursors through dynamic bonds to trigger the supramolecular assembly from small molecules in an aqueous solution is described. The supramolecular structures are crystalline in nature and the reaction coupled assembly strategy can be extended to a supramolecular assembly of aromatic amide derivatives formed in‐situ. The method may be instructive for the development of supramolecular nanocrystalline materials with desired physical properties.

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