Abstract

Cellulose nanofibrils (CNF) form hydrogels at low concentrations. These hydrogels are held together by transient interactions such as entanglement of fibrils, non-specific ionic interactions and hydrogen bonds; and are thus vulnerable for changes in the chemical environment or the influence of mechanical forces. By a covalent crosslinking of the fibrils, stable permanent gels can be formed. In this study we have produced CNF by using TEMPO mediated oxidation followed by fibrillation. During this procedure, carboxyl and aldehyde groups are introduced on the CNF surfaces. The aldehyde groups are suitable sites for crosslinking, as aldehydes readily form covalent bonds to primary amines through formation of Schiff bases. For this purpose the diamines ethylenediamine and hexamethylenediamine, differing with four carbon atoms in the chain, were used as crosslinker molecules. The results show that by varying the concentration and length of the crosslinker molecules, the elastic modulus of the gels could be controlled. The reversible gels were in this way transformed to irreversible gels by a simple water based reaction. Controlling gel strength is one important premise for the use of CNF in applications such as tissue engineering.

Highlights

  • Hydrogels are three-dimensional (3D) networks of mainly hydrophilic polymers capable of absorbing up to thousands times their own dry weight in water (Hoffman 2001; Seliktar 2012)

  • The aldehyde groups were utilized in the subsequent covalent crosslinking

  • In this work we demonstrate how reversible Cellulose nanofibrils (CNF) hydrogels, held together by fibril entanglement, ionic interactions and hydrogen bonds, can be transformed into permanent hydrogels by covalently linking the CNFs

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Summary

Introduction

Hydrogels are three-dimensional (3D) networks of mainly hydrophilic polymers capable of absorbing up to thousands times their own dry weight in water (Hoffman 2001; Seliktar 2012). In addition to the high water content of hydrogels, there is a range of other properties that are important for successful development of such applications, e.g. degradability in the human body, bioadhesion, bioactivity, transport through the network, and mechanical properties that should match those of native tissue (Seliktar 2012). The optimal mechanical properties for a cell niche vary as much as 300-fold from soft brain tissue (elastic modulus, E = 0.1 kPa) to rigid calcifying bone (E [ 30 kPa). It was proven that the matrix elasticity specified lineage towards neurons, myoblasts and osteoblasts. These results demonstrated how important it is to control the elasticity of the matrix in tissue engineering

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