Highly Oriented Bio‐Mimetic Hydrogels by Calendering

Abstract Anisotropic hydrogels are promising candidates as load‐bearing materials for tissue engineering, while huge challenges remain in exploring effective and scalable methods for the preparation of anisotropic hydrogels with simultaneous high tensile strength, large toughness, good fracture stra...

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Main Authors: Zhanqi Liu, Yuqing Wang, Haidi Wu, Huamin Li, Longcheng Tang, Guo Wang, Daxin Zhang, Jianping Yin, Yinggang Miao, Yongqian Shi, Pingan Song, An Xie, Xuewu Huang, Wancheng Gu, Yiu Wing Mai, Jiefeng Gao
Format: Article
Language:English
Published: Wiley 2025-08-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202504778
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author Zhanqi Liu
Yuqing Wang
Haidi Wu
Huamin Li
Longcheng Tang
Guo Wang
Daxin Zhang
Jianping Yin
Yinggang Miao
Yongqian Shi
Pingan Song
An Xie
Xuewu Huang
Wancheng Gu
Yiu Wing Mai
Jiefeng Gao
author_facet Zhanqi Liu
Yuqing Wang
Haidi Wu
Huamin Li
Longcheng Tang
Guo Wang
Daxin Zhang
Jianping Yin
Yinggang Miao
Yongqian Shi
Pingan Song
An Xie
Xuewu Huang
Wancheng Gu
Yiu Wing Mai
Jiefeng Gao
author_sort Zhanqi Liu
collection DOAJ
description Abstract Anisotropic hydrogels are promising candidates as load‐bearing materials for tissue engineering, while huge challenges remain in exploring effective and scalable methods for the preparation of anisotropic hydrogels with simultaneous high tensile strength, large toughness, good fracture strain, excellent fatigue and swelling resistances. Inspired by the brick‐and‐mortar layered structure of nacre and the hierarchical fibril strucure of soft tissues (e.g., tendon and ligament), a facile organogel‐assissted calendering strategy is reported to design anisotropic hydrogels with a highly oriented and dense fiber lamellar strucure. The synergy of shearing and annealing promotes macromolecular chain alignment and crystallinity along the calendering direction while forming a nacre‐like lamellar morphology in the thickness direction. The tensile strength, elastic modulus, toughness and fracture energy of the anisotropic hydrogels can reach as high as 41.0 ± 6.4 MPa, 67.0 ± 5.1 MPa, 46.2 ± 3.3 MJ m−3, and 62.20 ± 8.55 kJ m−2, respectively. More importantly, the hydrogels show excellent crack growth and swelling resistances with the fatigue threshold increased to 2170 J m−2. This study provides a promising approach for fabrication of large‐sized biomimetic anisotropic hydrogels with outstanding mechanical properties for biomedical and engineering applications.
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institution Kabale University
issn 2198-3844
language English
publishDate 2025-08-01
publisher Wiley
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series Advanced Science
spelling doaj-art-3d825befa92743daba82fe5b8d3a5feb2025-08-20T11:56:10ZengWileyAdvanced Science2198-38442025-08-011230n/an/a10.1002/advs.202504778Highly Oriented Bio‐Mimetic Hydrogels by CalenderingZhanqi Liu0Yuqing Wang1Haidi Wu2Huamin Li3Longcheng Tang4Guo Wang5Daxin Zhang6Jianping Yin7Yinggang Miao8Yongqian Shi9Pingan Song10An Xie11Xuewu Huang12Wancheng Gu13Yiu Wing Mai14Jiefeng Gao15School of Chemistry and Chemical Engineering Yangzhou University No 180, Road Siwangting Yangzhou Jiangsu 225002 ChinaSchool of Chemistry and Chemical Engineering Yangzhou University No 180, Road Siwangting Yangzhou Jiangsu 225002 ChinaSchool of Chemistry and Chemical Engineering Yangzhou University No 180, Road Siwangting Yangzhou Jiangsu 225002 ChinaSchool of Chemistry and Chemical Engineering Yangzhou University No 180, Road Siwangting Yangzhou Jiangsu 225002 ChinaKey Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education College of Material Chemistry and Chemical Engineering Hangzhou Normal University Hangzhou 311121 ChinaShanxi Key Laboratory of Impact Dynamics and its Engineering Application School of Aeronautics Northwestern Polytechnical University Xi'an 710072 ChinaShanxi Key Laboratory of Impact Dynamics and its Engineering Application School of Aeronautics Northwestern Polytechnical University Xi'an 710072 ChinaShanxi Key Laboratory of Impact Dynamics and its Engineering Application School of Aeronautics Northwestern Polytechnical University Xi'an 710072 ChinaShanxi Key Laboratory of Impact Dynamics and its Engineering Application School of Aeronautics Northwestern Polytechnical University Xi'an 710072 ChinaCollege of Environment and Safety Engineering Fuzhou University Fuzhou 350116 ChinaCentre for Future Materials University of Southern Queensland Springfield Campus Southern Queensland QLD 4300 AustraliaSchool of Chemistry and Chemical Engineering Yangzhou University No 180, Road Siwangting Yangzhou Jiangsu 225002 ChinaTesting Center Yangzhou University Yangzhou Jiangsu 225002 ChinaSchool of Chemistry and Chemical Engineering Yangzhou University No 180, Road Siwangting Yangzhou Jiangsu 225002 ChinaDepartment of Mechanical Engineering The Hong Kong Polytechnic University Hung Hom, Kowloon Hong Kong 999077 ChinaSchool of Chemistry and Chemical Engineering Yangzhou University No 180, Road Siwangting Yangzhou Jiangsu 225002 ChinaAbstract Anisotropic hydrogels are promising candidates as load‐bearing materials for tissue engineering, while huge challenges remain in exploring effective and scalable methods for the preparation of anisotropic hydrogels with simultaneous high tensile strength, large toughness, good fracture strain, excellent fatigue and swelling resistances. Inspired by the brick‐and‐mortar layered structure of nacre and the hierarchical fibril strucure of soft tissues (e.g., tendon and ligament), a facile organogel‐assissted calendering strategy is reported to design anisotropic hydrogels with a highly oriented and dense fiber lamellar strucure. The synergy of shearing and annealing promotes macromolecular chain alignment and crystallinity along the calendering direction while forming a nacre‐like lamellar morphology in the thickness direction. The tensile strength, elastic modulus, toughness and fracture energy of the anisotropic hydrogels can reach as high as 41.0 ± 6.4 MPa, 67.0 ± 5.1 MPa, 46.2 ± 3.3 MJ m−3, and 62.20 ± 8.55 kJ m−2, respectively. More importantly, the hydrogels show excellent crack growth and swelling resistances with the fatigue threshold increased to 2170 J m−2. This study provides a promising approach for fabrication of large‐sized biomimetic anisotropic hydrogels with outstanding mechanical properties for biomedical and engineering applications.https://doi.org/10.1002/advs.202504778anisotropic hydrogelscalenderingfatigue resistancemechanical properties
spellingShingle Zhanqi Liu
Yuqing Wang
Haidi Wu
Huamin Li
Longcheng Tang
Guo Wang
Daxin Zhang
Jianping Yin
Yinggang Miao
Yongqian Shi
Pingan Song
An Xie
Xuewu Huang
Wancheng Gu
Yiu Wing Mai
Jiefeng Gao
Highly Oriented Bio‐Mimetic Hydrogels by Calendering
Advanced Science
anisotropic hydrogels
calendering
fatigue resistance
mechanical properties
title Highly Oriented Bio‐Mimetic Hydrogels by Calendering
title_full Highly Oriented Bio‐Mimetic Hydrogels by Calendering
title_fullStr Highly Oriented Bio‐Mimetic Hydrogels by Calendering
title_full_unstemmed Highly Oriented Bio‐Mimetic Hydrogels by Calendering
title_short Highly Oriented Bio‐Mimetic Hydrogels by Calendering
title_sort highly oriented bio mimetic hydrogels by calendering
topic anisotropic hydrogels
calendering
fatigue resistance
mechanical properties
url https://doi.org/10.1002/advs.202504778
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