Citation: Tao Yuan, Jun-qi Sun. Polyelectrolyte Complexes-based Hydrogels with High Mechanical Strength and Excellent Self-recovery[J]. Acta Polymerica Sinica, ;2019, 50(12): 1263-1271. doi: 10.11777/j.issn1000-3304.2019.19093 shu

Polyelectrolyte Complexes-based Hydrogels with High Mechanical Strength and Excellent Self-recovery

Tao Yuan ,
Jun-qi Sun ^,

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012

Corresponding author: Jun-qi Sun, sun_junqi@jlu.edu.cn
Received Date: 5 May 2019
Revised Date: 13 July 2019

Polymeric hydrogels with high mechanical strength and excellent self-recovery are useful in tissue engineering, stretchable electronics and wearable devices. In this work, polyelectrolyte complexes-based hydrogels with high mechanical strength and excellent self-recovery are fabricated by complexation of poly(vinyl alcohol) modified with benzaldehyde-2,4-disulfonic acid disodium salt (BADS) (denoted as SPVA) with linear poly(ethylenimine) (LPEI) in aqueous solution followed by molding, drying and rehydration. The mechanical properties of the LPEI_a/x%-SPVA_b hydrogels, where x% represents the molar ratio of BADS to the monomer molar ratio of PVA, and a and b represent the feed mass ratio of LPEI to SPVA, can be well-tailored by varying the parameters such as the grafting ratio of BADS on SPVA and mass ratio of LPEI to SPVA. Stress-strain measurements indicate that the LPEI₁/18%-SPVA₁ hydrogels have the highest mechanical strength, with a tensile strength of ~ 10.0 MPa and a toughness of ~ 14.21 MJ/m³. A piece of the LPEI₁/18%-SPVA₁ hydrogel strip with a width of 2 mm and thickness of 2 mm can sequentially withstand various deformations such as bending, knotting, and twisting, and can lift a 1 kg weight without any damage. Besides the electrostatic interactions between sulfonate groups of SPVA and protonated amine groups of LPEI, Fourier transform infrared spectroscopy confirms the existence of hydrogen-bonding interactions between hydroxyl and sulfonate groups on SPVA. The synergy of strong electrostatic interactions and weak hydrogen-bonding interactions endows the hydrogels with high mechanical strength and toughness. Moreover, the hydrogels can completely recover from a strain of 200% to their original shape and mechanical properties within 1 h rest at room temperature without any external assistance. The excellent self-recovery of the LPEI₁/18%-SPVA₁ hydrogels originates from the high elastic retraction of polymer chains arising from electrostatic interactions and the reversibility of sacrificial hydrogen-bonding interactions. The high mechanical strength and excellent self-recovery will make the hydrogels have potential applications in aspects such as load-bearing materials, actuators and stretchable electronics.
- Hydrogels,
- Polyelectrolytes,
- Polyelectrolyte complexes,
- Self-recovery
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