Super-strong hydrogel reinforced by an interconnected hollow microfiber network via regulating the water-cellulose-copolymer interplay

Yifang Zhou; Junqing Chen; Ziyang Lu; Luhe Qi; Jie Zhou; Chao Xu; Lu Chen; Jing Huang; Sijun Wang; Zhiqiang Wang; Awais Ghani; Gang Tan; Cai Lu; Ze Liu; Zhenqian Pang; Hongbing Deng; Chaoji Chen

doi:10.1016/j.scib.2025.01.013

Super-strong hydrogel reinforced by an interconnected hollow microfiber network via regulating the water-cellulose-copolymer interplay

Sci Bull (Beijing). 2025 Jan 13:S2095-9273(25)00037-4. doi: 10.1016/j.scib.2025.01.013. Online ahead of print.

Authors

Yifang Zhou¹, Junqing Chen¹, Ziyang Lu¹, Luhe Qi¹, Jie Zhou¹, Chao Xu¹, Lu Chen¹, Jing Huang¹, Sijun Wang¹, Zhiqiang Wang¹, Awais Ghani², Gang Tan², Cai Lu³, Ze Liu³, Zhenqian Pang⁴, Hongbing Deng⁵, Chaoji Chen⁶

Affiliations

¹ Hubei Biomass-Resource Chemistry and Environmental Biotechnology Key Laboratory, Hubei Provincial Engineering Research Center of Emerging Functional Coating Materials, School of Resource and Environmental Sciences, Wuhan University, Wuhan 430079, China.
² Department of Architecture, College of Civil Engineering and Architecture, Zhejiang University, Hangzhou 310027, China; Smart Materials for Architecture Research Lab, Innovation Center of Yangtze River Delta, Zhejiang University, Jiaxing 314100, China.
³ Department of Engineering Mechanics, School of Civil Engineering, Wuhan University, Wuhan 430072, China.
⁴ Department of Architecture, College of Civil Engineering and Architecture, Zhejiang University, Hangzhou 310027, China; Smart Materials for Architecture Research Lab, Innovation Center of Yangtze River Delta, Zhejiang University, Jiaxing 314100, China. Electronic address: zqpang@zju.edu.cn.
⁵ Hubei Biomass-Resource Chemistry and Environmental Biotechnology Key Laboratory, Hubei Provincial Engineering Research Center of Emerging Functional Coating Materials, School of Resource and Environmental Sciences, Wuhan University, Wuhan 430079, China. Electronic address: hbdeng@whu.edu.cn.
⁶ Hubei Biomass-Resource Chemistry and Environmental Biotechnology Key Laboratory, Hubei Provincial Engineering Research Center of Emerging Functional Coating Materials, School of Resource and Environmental Sciences, Wuhan University, Wuhan 430079, China. Electronic address: chenchaojili@whu.edu.cn.

PMID: 39863486
DOI: 10.1016/j.scib.2025.01.013

Abstract

The discontinuous fiber reinforced hydrogels are easy to fail due to the fracture of the fiber matrix during load-bearing. Here, we propose a novel strategy based on the synergistic reinforcement of interconnected natural fiber networks at multiple scales to fabricate hydrogels with extraordinary mechanical properties. Specifically, the P(AA-AM)/Cel (P(AA-AM), poly(acrylic acid-acrylamide); Cel, cellulose) hydrogel is synthesized by copolymerizing AA and AM on a substrate of paper with an interconnected hollow cellulose microfiber network. This innovative design achieves a collaborative improvement of mechanical properties, including a 253-times increase in strength (27.8 vs. 0.11 MPa), 137-times increase in work of fracture (3.59 vs. 0.026 MJ m^-3), and 235-times increase in fracture energy (16.48 vs. 0.07 kJ m^-2). These outstanding mechanical properties benefit from the P(AA-AM) network formed by the copolymerization, which fills both the inside and outside of the hollow cellulose fibers, thus establishing abundant strong hydrogen bonds with the fibers and welding the fiber junctions. Consequently, the hydrogel exhibits enhanced resistance to the slippage and fracture of fibers. This strategy demonstrates the mechanical strengthening effectiveness of a variety of hydrogels by regulating the water-cellulose-copolymer interplay, representing a practical and universal route for designing super-strong hydrogels.

Keywords: Anti-freezing; Cellulose; Fiber reinforcement; Hydrogel; Hydrogen bond.