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<p>While hierarchical ordering is a distinctive feature of natural tissues and is directly responsible for their diverse and unique properties, efforts to synthesize biomaterials have primarily focused on using molecular-based approaches with little emphasis on multiscale structure. Here, we report a bottom-up self-assembly process to produce highly porous hydrogel fibers that resemble extracellular matrices both structurally and mechanically. Physically crosslinked nanostructured micelles form the walls of micrometer-sized water-rich pores with preferred orientation along the fiber direction. Low elastic moduli (&lt;1 kPa), high elasticity (extending by more than 12 times the initial length), non-linear elasticity (e.g., hyperelasticity), and completely reversible extension are derived from unevenly distributed strain between the micrometer-sized pores and the polymer chains, which is reminiscent of cellular solids. Control of the material microstructure and orientation over many orders of magnitude (e.g., nm–μm), while holding the nanostructure constant, reveals how the multiscale structure directly impacts mechanical properties.</p>

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Porous hierarchically ordered hydrogels demonstrating structurally dependent mechanical properties

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月23日

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  • Elisabeth C. Lloyd,
  • Sujata Dhakal,
  • Shahrouz Amini,
  • Rami Alhasan,
  • Peter Fratzl,
  • Douglas R. Tree,
  • Svetlana Morozova,
  • Robert J. Hickey

摘要

While hierarchical ordering is a distinctive feature of natural tissues and is directly responsible for their diverse and unique properties, efforts to synthesize biomaterials have primarily focused on using molecular-based approaches with little emphasis on multiscale structure. Here, we report a bottom-up self-assembly process to produce highly porous hydrogel fibers that resemble extracellular matrices both structurally and mechanically. Physically crosslinked nanostructured micelles form the walls of micrometer-sized water-rich pores with preferred orientation along the fiber direction. Low elastic moduli (<1 kPa), high elasticity (extending by more than 12 times the initial length), non-linear elasticity (e.g., hyperelasticity), and completely reversible extension are derived from unevenly distributed strain between the micrometer-sized pores and the polymer chains, which is reminiscent of cellular solids. Control of the material microstructure and orientation over many orders of magnitude (e.g., nm–μm), while holding the nanostructure constant, reveals how the multiscale structure directly impacts mechanical properties.