3D printable strong and tough composite organo-hydrogels inspired by natural hierarchical composite design principles

Quyang Liu, Xinyu Dong, Haobo Qi, Haoqi Zhang, Tian Li, Yijing Zhao, Guanjin Li and Wei Zhai ()
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Quyang Liu: National University of Singapore
Xinyu Dong: National University of Singapore
Haobo Qi: National University of Singapore
Haoqi Zhang: National University of Singapore
Tian Li: National University of Singapore
Yijing Zhao: National University of Singapore
Guanjin Li: National University of Singapore
Wei Zhai: National University of Singapore

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Fabrication of composite hydrogels can effectively enhance the mechanical and functional properties of conventional hydrogels. While ceramic reinforcement is common in many hard biological tissues, ceramic-reinforced hydrogels lack a similar natural prototype for bioinspiration. This raises a key question: How can we still attain bioinspired mechanical mechanisms in composite hydrogels without mimicking a specific composition and structure? Abstracting the hierarchical composite design principles of natural materials, this study proposes a hierarchical fabrication strategy for ceramic-reinforced organo-hydrogels, featuring (1) aligned ceramic platelets through direct-ink-write printing, (2) poly(vinyl alcohol) organo-hydrogel matrix reinforced by solution substitution, and (3) silane-treated platelet-matrix interfaces. Unit filaments are further printed into a selection of bioinspired macro-architectures, leading to high stiffness, strength, and toughness (fracture energy up to 31.1 kJ/m2), achieved through synergistic multi-scale energy dissipation. The materials also exhibit wide operation tolerance and electrical conductivity for flexible electronics in mechanically demanding conditions. Hence, this study demonstrates a model strategy that extends the fundamental design principles of natural materials to fabricate composite hydrogels with synergistic mechanical and functional enhancement.

Date: 2024
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DOI: 10.1038/s41467-024-47597-7

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