Microgel double-crosslinked hydrogel with excellent mechanical properties for flexible electronics.

Journal: Journal of colloid and interface science
Published Date: Jun 10, 2025

Abstract

Hydrogels are limited in practical applications due to insufficient mechanical properties. While microgels (MGs) and active MGs enhance hydrogel toughness via sacrificial bonding and chemical crosslinking, respectively, achieving synergistic multiple physical-chemical crosslinking remains challenging. In this study, pH-responsive soft MGs (PEA-MAA-BDDA) were synthesized as physical micro-crosslinkers, while vinyl-functionalized MGs (GMGs) were used as active MGs serving as chemical micro-crosslinkers. MGs and GMGs were dispersed in acrylamide (AAm) to prepare MGs physically crosslinked hydrogels (MPC-xMG), GMGs chemically crosslinked hydrogels (MCC-yGMG), and double micro-crosslinked hydrogels (MDC-xMG-yGMG). Mechanical performance is significantly affected by the micro-crosslinker content, pH, and crosslinking strategy, which regulate hydrogen bond strength, interparticle interactions, polymer chain entanglement, and crosslinking density. The dual crosslinked MDC hydrogels (MDC-1.0MG-0.3GMG) exhibited a synergistic balance of toughness and elasticity, resulting in exceptional stretchability and fracture resistance. Furthermore, incorporating carbon nanotubes (CNTs) yielded conductive hydrogels with excellent mechanical properties and ultralow hysteresis. These conductive hydrogels are suitable for flexible electronic skin, human motion monitoring, and real-time blood pressure prediction using long short-term memory (LSTM) neural networks. This work presents a programmable approach for designing mechanically robust hydrogels via pH-responsive dual micro-crosslinkers.

Authors

  • Yongyan Mo
    Dongguan Key Laboratory of Interdisciplinary Science for Advanced Materials and Large-Scale Scientific Facilities, School of Physical Sciences, Great Bay University, Dongguan, Guangdong 523000, PR China; Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong 518000, PR China.
  • Mingning Zhu
    School of Biomedical Engineering, Guangdong Medical University, Dongguan 523808, PR China; The First Dongguan Affiliated Hospital, Guangdong Medical University, Dongguan 523808, PR China. Electronic address: zhumn@gdmu.edu.cn.
  • Shuo Sun
    Laboratory of Biological Psychology, Department of Brain and Cognition, Leuven Brain Institute, Katholieke Universiteit Leuven, 3000 Leuven, Belgium.
  • Dazhi Sun
    Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong 518000, PR China. Electronic address: sundz@sustech.edu.cn.
  • Dongdong Lu
    Institute of Urology, The Third Affiliated Hospital of Shenzhen University, Shenzhen, 518000, P. R. China.

Keywords

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