Melt Densification Enables Fracture-resistant Blend Hydrogels

Melt Densification Enables Fracture-resistant Blend Hydrogels | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Melt Densification Enables Fracture-resistant Blend Hydrogels Xunan Hou, Zichun Zhu, Yuting Wen, Yixin Zhang, Chitinart Thedrattanawong, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6592950/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Hydrogels and elastomers are integral components in biomedical and electronics devices, but their toughness and crack resistance are often unsatisfactory for load-bearing applications. Synthetic polymer networks predominantly rely on solution fabrication, which compromises the ultimate mechanical properties. This work presents a universal melt crosslinking strategy, which densifies entanglements well beyond solvated conditions. When deformed, mutually entangled dissimilar chains stiffen the gels, while sparse crosslinks amplify fracture resistance. At water contents up to 83%, the resultant hydrogels demonstrate over 2 orders increase in mechanical properties, including moduli (1.3-35 MPa), toughness (0.7-24.5 kJ/m2) and fatigue thresholds (1.2-3.3 kJ/m2), tunable in a wide range beyond existing hydrogels. Furthermore, the hydrogels show high optical clarity (> 96%), oxygen permeability (Dk/t > 40) and anti-fouling properties (< 0.6μg cm-2). This generalizable strategy could guide the design of tough functional soft materials in fields such as healthcare and smart electronics. Physical sciences/Engineering/Mechanical engineering Physical sciences/Materials science/Soft materials/Gels and hydrogels Physical sciences/Engineering/Biomedical engineering Full Text Additional Declarations There is NO Competing Interest. Supplementary Files NatCommSMv3.pdf Supplementary info pdf file Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-6592950","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":457123343,"identity":"5141339f-c704-4491-b406-13ac1086e566","order_by":0,"name":"Xunan Hou","email":"","orcid":"https://orcid.org/0000-0002-7773-9300","institution":"National University of Singapore","correspondingAuthor":false,"prefix":"","firstName":"Xunan","middleName":"","lastName":"Hou","suffix":""},{"id":457123337,"identity":"948ec694-d898-41cc-b99d-b6472a7902fb","order_by":1,"name":"Zichun Zhu","email":"","orcid":"","institution":"National University of 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Synthetic polymer networks predominantly rely on solution fabrication, which compromises the ultimate mechanical properties. This work presents a universal melt crosslinking strategy, which densifies entanglements well beyond solvated conditions. When deformed, mutually entangled dissimilar chains stiffen the gels, while sparse crosslinks amplify fracture resistance. At water contents up to 83%, the resultant hydrogels demonstrate over 2 orders increase in mechanical properties, including moduli (1.3-35 MPa), toughness (0.7-24.5 kJ/m2) and fatigue thresholds (1.2-3.3 kJ/m2), tunable in a wide range beyond existing hydrogels. Furthermore, the hydrogels show high optical clarity (\u003e 96%), oxygen permeability (Dk/t \u003e 40) and anti-fouling properties (\u003c 0.6μg cm-2). 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