Abstract

Hydrogels have been extensively used in many fields. Current synthesis of functional hydrogels requires incorporation of functional molecules either before or during gelation via the pre-organized reactive site along the polymer chains within hydrogels, which is tedious for polymer synthesis and not flexible for different types of hydrogels. Inspired by sandcastle worm, we develop a simple one-step strategy to functionalize wet hydrogels using molecules bearing an adhesive dibutylamine-DOPA-lysine-DOPA tripeptide. This tripeptide can be easily modified with various functional groups to initiate diverse types of polymerizations and provide functional polymers with a terminal adhesive tripeptide. Such functional molecules enable direct modification of wet hydrogels to acquire biological functions such as antimicrobial, cell adhesion and wound repair. The strategy has a tunable functionalization degree and a stable attachment of functional molecules, which provides a tool for direct and convenient modification of wet hydrogels to provide them with diverse functions and applications.

Highlights

  • Hydrogels have been extensively used in many fields

  • Hydrogels can be prepared from a large variety of hydrophilic polymers including but not limited to polysaccharides (chitosan[16], sodium alginate (ALG)[17] etc.), poly(ethylene glycol) (PEG)[18], poly(vinyl alcohol) (PVA)[19], poly(2-hydroxyethyl methacrylate) (PHEMA)[20], poly(sulfobetaine methacrylate) (PSBMA)[21], and related polymers[22,23,24,25]

  • We demonstrated a convenient synthesis of this amine terminated DbaYKY through a solid-phase method (Supplementary Fig. 3), which enables other research groups and companies to obtain DbaYKY thereby greatly expanding its applications

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Summary

Introduction

Hydrogels have been extensively used in many fields. Current synthesis of functional hydrogels requires incorporation of functional molecules either before or during gelation via the pre-organized reactive site along the polymer chains within hydrogels, which is tedious for polymer synthesis and not flexible for different types of hydrogels. We develop a simple one-step strategy to functionalize wet hydrogels using molecules bearing an adhesive dibutylamine-DOPA-lysine-DOPA tripeptide This tripeptide can be modified with various functional groups to initiate diverse types of polymerizations and provide functional polymers with a terminal adhesive tripeptide. Adhesive materials have been extensively studied especially the mussel-inspired adhesive materials[33,34,35,36,37,38,39,40,41,42,43] Many of these studies use molecules that are terminally functionalized with 3,4-dihydroxy-L-phenylalanine (DOPA) or DOPA-lysine combinations to realize surface modifications[44,45,46,47,48,49]. The DbaYKY peptide enables direct modification of functional molecules to the surface and interior of hydrogels in an aqueous environment, providing hydrogels with diverse functions such as anti-bacteria, cell adhesion for tissue engineering, and wound healing (Fig. 1c)

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