Scholarlink

<p>Spider silks are exceptional biomaterials: biocompatible, biodegradable, and with remarkable mechanical properties. Unfortunately, attempts to replicate them tend to fail due to the difficulty of synthesizing the proteins that constitute them, and to an incomplete understanding of their processing conditions. Here, we report a synthetic system inspired by spider silk, consisting of a synthetic polyelectrolyte with grafted oligoalanine chains. We have used this peptide-polyelectrolyte conjugate to produce complex coacervates in an analogous process to the liquid-liquid phase separation (LLPS) observed during the natural processing of spider silk. We have characterized these coacervates using rheology, tack test, and solid-state NMR spectroscopy, observing α-helixes and <i>β</i>-sheets. These secondary structures crosslink the material, improving its mechanical properties and its processability, for example, for 3D printing. Furthermore, the peptide-based crosslinks cause distinctive behaviours – such as salt-induced aging. Our approach contributes to the fundamental understanding of the role that LLPS and peptide crosslinks play in spider silk, and to the development of new soft materials crosslinked by peptide aggregation.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Crosslinking, salt-induced aging, and secondary structure formation in Peptide-containing coacervates inspired by spider silk

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年8月28日

查看全文
  • Armin Amirsadeghi,
  • Raffaella Parlato,
  • Anna Kenbeek,
  • Ana Rita Gaspar,
  • Marta Oggioni,
  • Alessia Lasorsa,
  • Adrivit Mukherjee,
  • Malak Jaber,
  • Małgorzata K. Włodarczyk-Biegun,
  • Patrick C. A. van der Wel,
  • Marleen Kamperman,
  • Guillermo Monreal Santiago

摘要

Spider silks are exceptional biomaterials: biocompatible, biodegradable, and with remarkable mechanical properties. Unfortunately, attempts to replicate them tend to fail due to the difficulty of synthesizing the proteins that constitute them, and to an incomplete understanding of their processing conditions. Here, we report a synthetic system inspired by spider silk, consisting of a synthetic polyelectrolyte with grafted oligoalanine chains. We have used this peptide-polyelectrolyte conjugate to produce complex coacervates in an analogous process to the liquid-liquid phase separation (LLPS) observed during the natural processing of spider silk. We have characterized these coacervates using rheology, tack test, and solid-state NMR spectroscopy, observing α-helixes and β-sheets. These secondary structures crosslink the material, improving its mechanical properties and its processability, for example, for 3D printing. Furthermore, the peptide-based crosslinks cause distinctive behaviours – such as salt-induced aging. Our approach contributes to the fundamental understanding of the role that LLPS and peptide crosslinks play in spider silk, and to the development of new soft materials crosslinked by peptide aggregation.