Spatiotemporal toughness modulation in hydrogels through on-demand cross-linking

IF 12.5 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Science Advances Pub Date : 2025-10-10 DOI:10.1126/sciadv.adz0440

Jihun Lee, Rogerio M. Castilho, Sungmin Nam

{"title":"Spatiotemporal toughness modulation in hydrogels through on-demand cross-linking","authors":"Jihun Lee, Rogerio M. Castilho, Sungmin Nam","doi":"10.1126/sciadv.adz0440","DOIUrl":null,"url":null,"abstract":"<div >Tough hydrogels are promising for soft robotics, bioelectronics, and tissue adhesives due to their exceptional resilience and biocompatibility, yet precise spatiotemporal control of their mechanics remains challenging. Here, we present a hydrogel platform that enables spatiotemporal modulation of toughness through a latent ionic cross-linking mechanism. By embedding calcium carbonate (CaCO<sub>3</sub>) microparticles in alginate/polyacrylamide double-network hydrogels, we create a system where localized calcium release and thus ionic cross-linking can be programmed in both space and time. Spatial control is achieved by direct ink writing of CaCO<sub>3</sub>, while temporal activation is triggered by glucono-δ-lactone, a biocompatible acidifier that releases calcium on demand. This strategy allows user-defined tuning of stiffness and toughness, enabling fabrication of three-dimensional (3D) hydrogels with tailored mechanical profiles. The resulting materials offer a versatile platform for anisotropic impact shielding, directional strain sensing, and 3D-printed tissue adhesives, representing a paradigm shift for adaptive, reconfigurable, and multifunctional soft materials.</div>","PeriodicalId":21609,"journal":{"name":"Science Advances","volume":"11 41","pages":""},"PeriodicalIF":12.5000,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.science.org/doi/reader/10.1126/sciadv.adz0440","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science Advances","FirstCategoryId":"103","ListUrlMain":"https://www.science.org/doi/10.1126/sciadv.adz0440","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}

引用次数: 0

Abstract

Tough hydrogels are promising for soft robotics, bioelectronics, and tissue adhesives due to their exceptional resilience and biocompatibility, yet precise spatiotemporal control of their mechanics remains challenging. Here, we present a hydrogel platform that enables spatiotemporal modulation of toughness through a latent ionic cross-linking mechanism. By embedding calcium carbonate (CaCO₃) microparticles in alginate/polyacrylamide double-network hydrogels, we create a system where localized calcium release and thus ionic cross-linking can be programmed in both space and time. Spatial control is achieved by direct ink writing of CaCO₃, while temporal activation is triggered by glucono-δ-lactone, a biocompatible acidifier that releases calcium on demand. This strategy allows user-defined tuning of stiffness and toughness, enabling fabrication of three-dimensional (3D) hydrogels with tailored mechanical profiles. The resulting materials offer a versatile platform for anisotropic impact shielding, directional strain sensing, and 3D-printed tissue adhesives, representing a paradigm shift for adaptive, reconfigurable, and multifunctional soft materials.

Abstract Image

查看原文本刊更多论文

通过按需交联调节水凝胶的时空韧性

由于其特殊的弹性和生物相容性，坚韧的水凝胶在软机器人、生物电子学和组织粘合剂方面很有前景，但对其力学的精确时空控制仍然具有挑战性。在这里，我们提出了一个水凝胶平台，可以通过潜在的离子交联机制对韧性进行时空调节。通过将碳酸钙（caco3）微粒嵌入海藻酸盐/聚丙烯酰胺双网络水凝胶中，我们创建了一个系统，在该系统中，局部钙释放和离子交联可以在空间和时间上进行编程。空间控制是通过caco3的直接墨水书写实现的，而时间激活是由葡萄糖-δ-内酯触发的，葡萄糖-δ-内酯是一种生物相容性酸化剂，可以根据需要释放钙。该策略允许用户自定义调整刚度和韧性，从而实现具有定制机械轮廓的三维（3D）水凝胶的制造。由此产生的材料为各向异性冲击屏蔽、定向应变传感和3d打印组织粘合剂提供了一个通用的平台，代表了自适应、可重构和多功能软材料的范式转变。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Science Advances 综合性期刊-综合性期刊

CiteScore

21.40

自引率

1.50%

发文量

1937

审稿时长

29 weeks

期刊介绍： Science Advances, an open-access journal by AAAS, publishes impactful research in diverse scientific areas. It aims for fair, fast, and expert peer review, providing freely accessible research to readers. Led by distinguished scientists, the journal supports AAAS's mission by extending Science magazine's capacity to identify and promote significant advances. Evolving digital publishing technologies play a crucial role in advancing AAAS's global mission for science communication and benefitting humankind.