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<p>Bio-based conductive hydrogels have garnered significant attention in flexible wearable sensors due to their exceptional biocompatibility, flexibility, and sensing capabilities. Nevertheless, achieving simultaneous improvements in mechanical robustness, competitive conductivity, and high sensing sensitivity remained a critical challenge in hydrogel design. This study proposed a nanocellulose-enhanced double-network (DN) strategy by incorporating electrostatic-interactive TEMPO-oxidized cellulose nanofibers (TOCNFs) and cationic cellulose nanofibrils (C-CNFs) into a polyvinyl alcohol (PVA) matrix, synergized with LiCl for ionic conductivity enhancement. The hierarchical architecture featured a TOCNF/C-CNF electrostatic network as one of the networks and PVA-based hydrogen-bonded network as another, creating an all-physical-crosslinked PVA/C-CNF/TOCNF (PCT) hydrogel through multivalent hydrogen bonding and Coulombic interactions. This nanocellulose-driven DN configuration enabled extraordinary integrated performance for the optimized PCT3 hydrogel, including ultrahigh tensile strength (2.1&#xa0;MPa) with 527% elongation, remarkable ionic conductivity (2.63&#xa0;S/m), and a maximum gauge factor (GF) of 14.188. Notably, TOCNF-C-CNF ionic complementarity enhanced electrostatic networks and created ion-transport channels, enabling mechanical–electrical synergy superior to most biobased hydrogels. The PCT hydrogel demonstrated superior motion sensing capabilities spanning macroscopic joint movements to subtle muscle vibrations. This nanocellulose-engineered hydrogel demonstrated transformative potential for next-generation wearable electronics, leveraging inherent biocompatibility and eco-friendly processing to establish a sustainable paradigm for high-performance sensors through nanocellulose network modulation.</p>

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Nanocellulose interlocking architectonics meets green hydrogel: high-performance wearable electronics

  • 期刊论文

  • 发表日期：

    2026年4月6日

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  • Xinyi Li,
  • Jianbo Huang,
  • Lijun Zhao,
  • Yue Xu,
  • Hongkai Li,
  • Lumen Chao,
  • Yang Yang,
  • Wen Liu,
  • Xiaoying Wang

摘要

Bio-based conductive hydrogels have garnered significant attention in flexible wearable sensors due to their exceptional biocompatibility, flexibility, and sensing capabilities. Nevertheless, achieving simultaneous improvements in mechanical robustness, competitive conductivity, and high sensing sensitivity remained a critical challenge in hydrogel design. This study proposed a nanocellulose-enhanced double-network (DN) strategy by incorporating electrostatic-interactive TEMPO-oxidized cellulose nanofibers (TOCNFs) and cationic cellulose nanofibrils (C-CNFs) into a polyvinyl alcohol (PVA) matrix, synergized with LiCl for ionic conductivity enhancement. The hierarchical architecture featured a TOCNF/C-CNF electrostatic network as one of the networks and PVA-based hydrogen-bonded network as another, creating an all-physical-crosslinked PVA/C-CNF/TOCNF (PCT) hydrogel through multivalent hydrogen bonding and Coulombic interactions. This nanocellulose-driven DN configuration enabled extraordinary integrated performance for the optimized PCT3 hydrogel, including ultrahigh tensile strength (2.1 MPa) with 527% elongation, remarkable ionic conductivity (2.63 S/m), and a maximum gauge factor (GF) of 14.188. Notably, TOCNF-C-CNF ionic complementarity enhanced electrostatic networks and created ion-transport channels, enabling mechanical–electrical synergy superior to most biobased hydrogels. The PCT hydrogel demonstrated superior motion sensing capabilities spanning macroscopic joint movements to subtle muscle vibrations. This nanocellulose-engineered hydrogel demonstrated transformative potential for next-generation wearable electronics, leveraging inherent biocompatibility and eco-friendly processing to establish a sustainable paradigm for high-performance sensors through nanocellulose network modulation.