Resolving hyperelasticity-adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneities

Abstract Stretchable materials with low hysteresis and strong adhesion are needed in applications, but unifying the two contradictory mechanical properties is challenging. Herein, we propose the design principles of polymer networks that are hyperelastic yet adhesive by rationalizing mechanical hete...

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Main Authors: Ping Zhang, Haowei Ruan, Qingxian Li, Yunfeng He, Canhui Yang
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-61450-5
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author Ping Zhang
Haowei Ruan
Qingxian Li
Yunfeng He
Canhui Yang
author_facet Ping Zhang
Haowei Ruan
Qingxian Li
Yunfeng He
Canhui Yang
author_sort Ping Zhang
collection DOAJ
description Abstract Stretchable materials with low hysteresis and strong adhesion are needed in applications, but unifying the two contradictory mechanical properties is challenging. Herein, we propose the design principles of polymer networks that are hyperelastic yet adhesive by rationalizing mechanical heterogeneities. The heterogeneous networks comprise a viscoelastic adhesive surface and a hyperelastic non-adhesive bulk. The former has a stiffness much smaller than that of the latter. We synthesize the networks by harnessing the oxygen inhibition mechanism, construct a polymerization phase diagram by reconciling the kinetics of polymerization and radical quenching of oxygen, and establish a power law criterion for the transition from a viscoelastic adhesive network to a hyperelastic adhesive network. We illustrate the principle with heterogeneous poly(butyl acrylate-co-acrylic acid) networks, achieving hysteresis <5% and adhesion energy >300 J/m2. We show that the adhesion energy-thickness relation of hyperelastic adhesive polymer networks is nonlinear below a transition thickness. Hyperelastic and adhesive stretchable materials potentialize high-cycle and fatigue-resistant soft human-machine interfaces and beyond.
format Article
id doaj-art-53b3d5008d734c78a1d2cf7463cb32c3
institution Kabale University
issn 2041-1723
language English
publishDate 2025-07-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj-art-53b3d5008d734c78a1d2cf7463cb32c32025-08-20T04:01:41ZengNature PortfolioNature Communications2041-17232025-07-0116111110.1038/s41467-025-61450-5Resolving hyperelasticity-adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneitiesPing Zhang0Haowei Ruan1Qingxian Li2Yunfeng He3Canhui Yang4Shenzhen Key Laboratory of Soft Mechanics & Smart Manufacturing, Department of Mechanics and Aerospace Engineering, Southern University of Science and TechnologyShenzhen Key Laboratory of Soft Mechanics & Smart Manufacturing, Department of Mechanics and Aerospace Engineering, Southern University of Science and TechnologyShenzhen Key Laboratory of Soft Mechanics & Smart Manufacturing, Department of Mechanics and Aerospace Engineering, Southern University of Science and TechnologyShenzhen Key Laboratory of Soft Mechanics & Smart Manufacturing, Department of Mechanics and Aerospace Engineering, Southern University of Science and TechnologyShenzhen Key Laboratory of Soft Mechanics & Smart Manufacturing, Department of Mechanics and Aerospace Engineering, Southern University of Science and TechnologyAbstract Stretchable materials with low hysteresis and strong adhesion are needed in applications, but unifying the two contradictory mechanical properties is challenging. Herein, we propose the design principles of polymer networks that are hyperelastic yet adhesive by rationalizing mechanical heterogeneities. The heterogeneous networks comprise a viscoelastic adhesive surface and a hyperelastic non-adhesive bulk. The former has a stiffness much smaller than that of the latter. We synthesize the networks by harnessing the oxygen inhibition mechanism, construct a polymerization phase diagram by reconciling the kinetics of polymerization and radical quenching of oxygen, and establish a power law criterion for the transition from a viscoelastic adhesive network to a hyperelastic adhesive network. We illustrate the principle with heterogeneous poly(butyl acrylate-co-acrylic acid) networks, achieving hysteresis <5% and adhesion energy >300 J/m2. We show that the adhesion energy-thickness relation of hyperelastic adhesive polymer networks is nonlinear below a transition thickness. Hyperelastic and adhesive stretchable materials potentialize high-cycle and fatigue-resistant soft human-machine interfaces and beyond.https://doi.org/10.1038/s41467-025-61450-5
spellingShingle Ping Zhang
Haowei Ruan
Qingxian Li
Yunfeng He
Canhui Yang
Resolving hyperelasticity-adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneities
Nature Communications
title Resolving hyperelasticity-adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneities
title_full Resolving hyperelasticity-adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneities
title_fullStr Resolving hyperelasticity-adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneities
title_full_unstemmed Resolving hyperelasticity-adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneities
title_short Resolving hyperelasticity-adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneities
title_sort resolving hyperelasticity adhesiveness conflict in polymer networks by in situ constructing mechanical heterogeneities
url https://doi.org/10.1038/s41467-025-61450-5
work_keys_str_mv AT pingzhang resolvinghyperelasticityadhesivenessconflictinpolymernetworksbyinsituconstructingmechanicalheterogeneities
AT haoweiruan resolvinghyperelasticityadhesivenessconflictinpolymernetworksbyinsituconstructingmechanicalheterogeneities
AT qingxianli resolvinghyperelasticityadhesivenessconflictinpolymernetworksbyinsituconstructingmechanicalheterogeneities
AT yunfenghe resolvinghyperelasticityadhesivenessconflictinpolymernetworksbyinsituconstructingmechanicalheterogeneities
AT canhuiyang resolvinghyperelasticityadhesivenessconflictinpolymernetworksbyinsituconstructingmechanicalheterogeneities