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<p>Polymer gels are widely utilized in biomedical applications such as drug delivery, tissue engineering scaffolds, and wound dressings, where their surfaces directly interface with living systems. While extensive research has been devoted to solid polymer surfaces with nanoscale control, systematic investigations of gel surfaces have been relatively limited. This review highlights self-organized structures emerging at gel surfaces, including skin layers, shrinkage- and wrinkle-type patterns, and phase-separated structures, which critically influence both interfacial and bulk properties. Historical studies from the 1980s and 1990s revealed diverse structural phenomena, yet uncertainties in their occurrence, often depending on chemical composition and systematic regulation, remain unresolved. Recent advances, particularly surface grafting techniques employing living radical polymerization, have enabled enforced induction and controlled design of such structures at multiple spatial scales. These insights establish a new perspective on the structure–property relationships of gels, emphasizing the interplay between the surface and bulk. Beyond fundamental understanding, this concept has broad implications for the rational design of advanced biomaterials.</p>

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Self-organized structures at polymer gel surfaces: Mechanisms, controlled design, and perspectives

  • 期刊论文

  • 发表日期：

    2025年12月4日

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  • Aya M. Akimoto

摘要

Polymer gels are widely utilized in biomedical applications such as drug delivery, tissue engineering scaffolds, and wound dressings, where their surfaces directly interface with living systems. While extensive research has been devoted to solid polymer surfaces with nanoscale control, systematic investigations of gel surfaces have been relatively limited. This review highlights self-organized structures emerging at gel surfaces, including skin layers, shrinkage- and wrinkle-type patterns, and phase-separated structures, which critically influence both interfacial and bulk properties. Historical studies from the 1980s and 1990s revealed diverse structural phenomena, yet uncertainties in their occurrence, often depending on chemical composition and systematic regulation, remain unresolved. Recent advances, particularly surface grafting techniques employing living radical polymerization, have enabled enforced induction and controlled design of such structures at multiple spatial scales. These insights establish a new perspective on the structure–property relationships of gels, emphasizing the interplay between the surface and bulk. Beyond fundamental understanding, this concept has broad implications for the rational design of advanced biomaterials.