Abstract

Gelation kinetics of hydrogels is closely linked to many applications such as the development of injectable and printable hydrogels. However, the control of gelation kinetics without compromising the structure and other properties of the hydrogels, remains a challenge. Here, we demonstrate a method to control the gelation kinetics of cucurbit[7]uril-adamantane (CB[7]-AD) cross-linked supramolecular hydrogels by using competing guest molecules. The association between CB[7] and AD moieties on the polymer backbone was impeded by pre-occupying the CB[7] cavity with competing guest molecules. By using various guest molecules and concentrations, the gelation of the hydrogels could be varied from seconds to hours. The strong interaction of CB[7]-AD pair endue the hydrogels good mechanical properties and stability. Moreover, the binding of functionalized guest molecules of CB[7] moieties offers a facile approach for tailoring of the hydrogels’ scaffold. Combined with hydrogel injection and printing technology, this method offers an approach for the development of hydrogels with advanced temporal and spatial complexity.

Highlights

  • Gelation kinetics of hydrogels is closely linked to many applications such as the development of injectable and printable hydrogels

  • There is unmet need for gelation mechanisms with controllable gelation kinetics which are independent of other properties

  • Numerous competing guest molecules can be employed in the control of certain CB based host-guest interactions, which offer a wide range of interaction dynamics

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Summary

Introduction

Gelation kinetics of hydrogels is closely linked to many applications such as the development of injectable and printable hydrogels. We demonstrate a method to control the gelation kinetics of cucurbit[7]uril-adamantane (CB[7]-AD) cross-linked supramolecular hydrogels by using competing guest molecules. Consisting of methylene bridged glycolurils, these pumpkin shaped, rigid molecules demonstrate amazing binding affinity and selectivity to a wide range of guest molecules27–29 With such binding properties, numerous competing guest molecules can be employed in the control of certain CB based host-guest interactions, which offer a wide range of interaction dynamics. The supramolecular inherence allows the hydrogels to be decorated with functional groups through host-guest interactions Based on these features, the hydrogels were demonstrated applicable for both of the injection and printing operation with good strength and tailorable properties

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