Arresting Microphase Separation Encodes Material Mechanics by Sculpting Microarchitectures and Local Polymer Enrichment
Abstract
Abstract Mechanical properties are central to material functionality. Although aqueous two‐phase systems (ATPS) can generate microarchitectures in soft materials such as hydrogels, their influence on mechanics, particularly toughness and energy dissipation, remains poorly understood. Here, diverse microarchitectures are systematically engineered within materials via ATPS‐induced local polymer enrichment, which yielding inverse globular, globular, and spinodal patterns, and revealing that each microarchitecture exhibits distinct mechanical behaviors. Most notably, spinodal hydrogel designs improve load distribution, increase fracture resistance, and promote efficient energy dissipation. These insights are used to develop and introduce single polymer phase separation (SPPS) as an innovative strategy to sculpt microarchitectures by tuning the ionic concentration, which overcomes traditional limitations of dual polymer systems. This novel approach enables scalable, low‐complexity, and chemically clean control over stiffness, toughness, and energy dissipation, independent of secondary polymers. Beyond mechanical advantages, spinodal architectures also support enhanced cell migration and biological activity. These findings demonstrate that microarchitectural design, rather than total polymer composition alone, dictates hydrogel mechanics. ATPS and SPPS provide robust and scalable methods to encode distinct mechanical and functional properties via microarchitecture variations into hydrogels, opening opportunities across tissue engineering, biofabrication, soft electronics, and food engineering.
Article Details
Authors (10)
Castro Johnbosco
Leijten Laboratory Department of BioEngineering Technologies TechMed Centre Faculty of Science and Technology University of Twente Enschede 7500AE The Netherlands
Floris Dalenoord
Leijten Laboratory Department of BioEngineering Technologies TechMed Centre Faculty of Science and Technology University of Twente Enschede 7500AE The Netherlands
Jarno Hiemstra
Leijten Laboratory Department of BioEngineering Technologies TechMed Centre Faculty of Science and Technology University of Twente Enschede 7500AE The Netherlands
Yu Na
Leijten Laboratory Department of BioEngineering Technologies TechMed Centre Faculty of Science and Technology University of Twente Enschede 7500AE The Netherlands
Alexis Wolfel
Leijten Laboratory Department of BioEngineering Technologies TechMed Centre Faculty of Science and Technology University of Twente Enschede 7500AE The Netherlands
Cécile Bosmans
Leijten Laboratory Department of BioEngineering Technologies TechMed Centre Faculty of Science and Technology University of Twente Enschede 7500AE The Netherlands
Christine Gering
Leijten Laboratory Department of BioEngineering Technologies TechMed Centre Faculty of Science and Technology University of Twente Enschede 7500AE The Netherlands
Niels Willemen
Leijten Laboratory Department of Bioengineering Technologies Faculty of Science and Technology TechMed Centre University Twente Enschede Netherlands
Su Ryon Shin
Division of Engineering in Medicine Department of Medicine Brigham and Women's Hospital Harvard Medical School Cambridge Massachusetts USA
Jeroen Leijten
Leijten Laboratory Department of Bioengineering Technologies Faculty of Science and Technology TechMed Centre University Twente Enschede Netherlands