Abstract

Tough and antimicrobial dual-crosslinked poly((trimethylamino)ethyl methacrylate chloride)-phytic acid hydrogel (pTMAEMA-PA) has been synthesized by adding a chemical crosslinker and docking a physical crosslinker of multivalent phytic acid into a cationic polyelectrolyte network. By increasing the loading concentration of PA, the tough hydrogel exhibits compressive stress of >1 MPa, along with high elasticity and fatigue-resistant properties. The enhanced mechanical properties of pTMAEMA-PA stem from the multivalent ion effect of PA via the formation of ion bridges within polyelectrolytes. In addition, a comparative study for a series of pTMAEMA-counterion complexes was conducted to elaborate the relationship between swelling ratio and mechanical strength. The study also revealed secondary factors, such as ion valency, ion specificity and hydrogen bond formation, holding crucial roles in tuning mechanical properties of the polyelectrolyte hydrogel. Furthermore, in bacteria attachment and disk diffusion tests, pTMAEMA-PA exhibits superior fouling resistance and antibacterial capability. The results reflect the fact that PA enables chelating strongly with divalent metal ions, hence, disrupting the outer membrane of bacteria, as well as dysfunction of organelles, DNA and protein. Overall, the work demonstrated a novel strategy for preparation of tough polyelectrolyte with antibacterial capability via docking PA to open up the potential use of PA in medical application.

Highlights

  • Hydrogels, a three-dimensional polymer network with high water content, has been extensively applied in biomedical applications, including tissue engineering scaffolds, tissue adhesives, drug delivery system, soft robotics, biosensors, and electronic components [1]

  • Was 24.5 ± 5 kPa and 29.9% ± 4%, respectively, which are much lower than poly((trimethylamino)ethyl methacrylate chloride) (pTMAEMA)-phytic acid (PA)-1

  • The fatigue resistant properties of pTMAEMA-PA-1 were further evaluated by the cyclic compressive test

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Summary

Introduction

A three-dimensional polymer network with high water content, has been extensively applied in biomedical applications, including tissue engineering scaffolds, tissue adhesives, drug delivery system, soft robotics, biosensors, and electronic components [1]. Inspired by the compelling characteristics of a plant-based protocatechualdehyde in the formation of imide and coordinative bonds, Cheng0 s group has recently introduced a novel approach to fabricate a supramolecular multistimuli-responsive hydrogel with antibacterial capability [32] Another plant derivative, phytic acid (PA) has been broadly applied in a variety of purposes, ranging from enhancing mechanical properties of materials [33,34] to therapeutic uses such as anticancer drug [35]. Based on previous findings [27,37,42], we proposed a novel dual-crosslinked pTMAEMA hydrogel obtaining both high fracture strength and antimicrobial capability by promoting non-covalent interaction between quaternary ammonium headgroups of pTMAEMA and multivalent-anionic PA. Staphylococcus epidermidis (S. epidermidis) were used in bacterial adhesion test and antibacterial diffusion test

Materials
Preparation of Polycationic Hydrogels
Compressive Mechanical Test
Rheological Test
Stability Test
Swelling Ratio Measurement
Bacterial Attachment Test
Antibacterial Activity
The Effect of Loading Concentration of PA on Mechanical Properties of pTMAEMA
The Fatigue-Resistant Properties and Self-Recovery of pTMAEMA-PA
Counterion
FTIR Analysis
Bacterial Attachment Test of pTMAEMA-Counterions
Antibacterial Capability of pTMAEMA-PA
Conclusions
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