Abstract
Hyaluronic acid (HA) and gelatin (Gel) are major components of the extracellular matrix of different tissues, and thus are largely appealing for the construction of hybrid hydrogels to combine the favorable characteristics of each biopolymer, such as the gel adhesiveness of Gel and the better mechanical strength of HA, respectively. However, despite previous studies conducted so far, the relationship between composition and scaffold structure and physico-chemical properties has not been completely and systematically established. In this work, pure and hybrid hydrogels of methacroyl-modified HA (HAMA) and Gel (GelMA) were prepared by UV photopolymerization and an extensive characterization was done to elucidate such correlations. Methacrylation degrees of ca. 40% and 11% for GelMA and HAMA, respectively, were obtained, which allows to improve the hydrogels’ mechanical properties. Hybrid GelMA/HAMA hydrogels were stiffer, with elastic modulus up to ca. 30 kPa, and porous (up to 91%) compared with pure GelMA ones at similar GelMA concentrations thanks to the interaction between HAMA and GelMA chains in the polymeric matrix. The progressive presence of HAMA gave rise to scaffolds with more disorganized, stiffer, and less porous structures owing to the net increase of mass in the hydrogel compositions. HAMA also made hybrid hydrogels more swellable and resistant to collagenase biodegradation. Hence, the suitable choice of polymeric composition allows to regulate the hydrogels´ physical properties to look for the most optimal characteristics required for the intended tissue engineering application.
Highlights
Tissue engineering (TE) has emerged in the last two decades to address the scarce availability of donors for patients who require a new organ or tissue after failure caused by a disease or trauma [1]
The methacrylation process involved the addition of a methacryloyl group to the amine and hydroxyl residues of Gel and Hyaluronic acid (HA) [33,34]
The amount of photo-initiator used for photopolymerization was adjusted to the number of double bonds in Gel and HA polymeric chains
Summary
Tissue engineering (TE) has emerged in the last two decades to address the scarce availability of donors for patients who require a new organ or tissue after failure caused by a disease or trauma [1] These “synthetic” alternatives can be engineered from a wide combination of different materials able to provide scaffolds to support cell adhesion and a suitable microenvironment for cell proliferation, organization, and subsequent tissue regeneration [2,3,4,5]. Among the different types of materials to construct scaffolds for TE, hydrogels play a key role These are three-dimensional cross-linked networks of polymers, proteins, and/or peptides [6] able to absorb and maintain large quantities of water inside without being dissolved thanks to their numerous hydrophilic groups, which allow extensive inner chemical and/or physical bonding. The composition and mechanical properties of synthetized hydrogels greatly influence biological cell responses in vitro and in vivo because cells sense the nano/microtopography and the biochemical anchoring points or receptors present in the formed bio-polymeric matrices; besides, adhered cells are influenced by the rigidity/softness of the scaffold, modulating their motility, proliferation, differentiation, and apoptosis responses [8,9,10]
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