Cellulose nanofibril-guided orienting response of supramolecular network enables superstretchable, robust, and antifatigue hydrogel

Siheng Wang; Le Yu; Xiangzheng Jia; Lei Zhang; He Liu; Enlai Gao; Chaoji Chen

doi:10.59717/j.xinn-mater.2024.100092

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Cellulose nanofibril-guided orienting response of supramolecular network enables superstretchable, robust, and antifatigue hydrogel

1.
Key Laboratory of Biomass Energy and Material, Jiangsu Province; Key Laboratory of Chemical Engineering of Forest Products, National Forestry and Grassland Administration; National Engineering Research Center of Low-Carbon Processing and Utilization of Forest Biomass; Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry, Nanjing 210042, China
2.
Hubei Biomass-Resource Chemistry and Environmental Biotechnology Key Laboratory, School of Resource and Environmental Sciences, Wuhan University, Wuhan 430079, China
3.
Department of Engineering Mechanics, School of Civil Engineering, Wuhan University, Wuhan 430072, China
4.
These authors contributed equally

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Corresponding authors: liuhe.caf@gmail.com (H.L.); enlaigao@whu.edu.cn (E.G.); chenchaojili@whu.edu.cn (C.C.);
Received Date: 27 June 2024

Accepted Date: 19 September 2024

Published Online: 24 September 2024

The Innovation Materials https://doi.org/10.59717/j.xinn-mater.2024.100092 | Cite this article

GRAPHICAL ABSTRACT

GRAPHICAL ABSTRACT

PUBLIC SUMMARY

PUBLIC SUMMARY
1. The high-performance hydrogel is constructed via cellulose nanofibril-guided orienting response of network.
  
  The supramolecular assembly process of cellulosic network from isotropic to aligned structure is revealed.
  
  The enabling hydrogel combines superstretchability, ultrarobustness, and fatigue-resistance.

ABSTRACT

ABSTRACT

Hydrogels featuring randomly networked matrix typically show poor mechanical strength owing to the weak interchain interactions of the matrix. Encouragingly, the stretchability and toughness of hydrogel materials along a certain direction were recently improved to an unprecedented level with the design of structured and oriented matrix, the realization of excellent and concurrently isotropic mechanical performance for hydrogels now become the next- research goal. Herein, a self-assembling process of poly(vinyl alcohol) (PVA) macromolecular chain and cellulose nanofibril (CNF) induced by the salting-out effect was reported, which allowed the formation of a strongly hydrogen-bonded PVA-CNF supramolecular matrix. The resulting hydrogel, in any direction, can show an ultra-high stretchability of 7,400% and a true tensile strength of 420 MPa through the orientation of the supramolecular matrix. The robustness of the supramolecular interaction between PVA and CNF was experimentally demonstrated by the fact that the hydrogel showed a high fracture energy (reaching up to 95.7 kJ m⁻²) and low notch sensitivity (fatigue threshold of 3,203 J m⁻²), even outperforming most state-of-the-art anisotropic hydrogels. These results highlight that constructing supramolecular interaction among various components of gel matrix holds great promise for the design of future gel materials with the extraordinary mechanical performance.
- cellulose nanofibrils /
- supramolecular assembly /
- biomass /
- superstretchable hydrogels /
- antifatigue hydrogels

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Wang S., Yu L., Jia X., et al., (2024). Cellulose nanofibril-guided orienting response of supramolecular network enables superstretchable, robust, and antifatigue hydrogel. The Innovation Materials 2(4): 100092. https://doi.org/10.59717/j.xinn-mater.2024.100092

Wang S., Yu L., Jia X., et al., (2024). Cellulose nanofibril-guided orienting response of supramolecular network enables superstretchable, robust, and antifatigue hydrogel. The Innovation Materials 2(4): 100092. https://doi.org/10.59717/j.xinn-mater.2024.100092

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