Porous Poly(2-hydroxyethyl methacrylate) Hydrogel Scaffolds for Tissue Engineering: Influence of Crosslinking Systems and Silk Sericin Concentration on Scaffold Properties

Abstract

Tailored porous structures of poly(2-hydroxyethyl methacrylate) (PHEMA) and silk sericin (SS) were used to create porous hydrogel scaffolds using two distinct crosslinking systems. These structures were designed to closely mimic the porous nature of the native extracellular matrix. Conventional free radical polymerization of 2-hydroxyethyl methacrylate (HEMA) was performed in the presence of different concentrations of SS (1.25, 2.50, 5.00% w/v) with two crosslinking systems. A chemical crosslinking system with N’N-methylene bisacrylamide (MBAAm) and a physical crosslinking system with dimethylurea (DMU) were used: C-PHEMA/SS (crosslinked using MBAAm) and C-PHEMA/pC-SS (crosslinked using MBAAm and DMU). The focus of this study was on investigating the impact of these crosslinking methods on various properties of the scaffolds, including pore size, pore characteristics, polymerization time, morphology, molecular interaction, in vitro degradation, thermal properties, and in vitro cytotoxicity. The various crosslinked networks were found to appreciably influence the properties of the scaffolds, especially the pore sizes, in which smaller sizes and higher numbers of pores with high regularity were seen in C-PHEMA/1.25 pC-SS (17 ± 2 μm) than in C-PHEMA/1.25 SS (34 ± 3 μm). Semi-interpenetrating networks were created by crosslinking PHEMA-MBAAm-PHEMA while incorporating free protein molecules of SS within the networks. The additional crosslinking step involving DMU occurred through hydrogen bonding of the -C=O and -N-H groups with the SS, resulting in the simultaneous incorporation of DMU and SS within the PHEMA networks. As a consequence of this process, the scaffold C-PHEMA/pC-SS exhibited smaller pore sizes compared to scaffolds without DMU crosslinking. Moreover, the incorporation of higher loadings of SS led to even smaller pore sizes. Additionally, the gelation time of C-PHEMA/pC-SS was delayed due to the presence of DMU in the crosslinking system. Both porous hydrogel scaffolds, C-PHEMA/pC-SS and PHEMA, were found to be non-cytotoxic to the normal human skin dermal fibroblast cell line (NHDF cells). This promising result indicates that these hydrogel scaffolds have potential for use in tissue engineering applications.

Utilizing Silk Sericin as a Biomaterial for Drug Encapsulation in a Hydrogel Matrix with Polycaprolactone: Formulation and Evaluation of Antibacterial Activity

“…Ekasurya et al crafted an SS/PVA hydrogel specifically for diabetic foot ulcer treatment, showcasing its capability to regenerate skin tissue . Tuancharoensri et al engineered an SS/PHEMA hydrogel scaffold for tissue engineering, offering insights into tailoring hydrogel properties for potential use in skin tissue regeneration within tissue engineering contexts . Critical literature review on the development of sericin-based hydrogels was conducted by different aspects such as type and nature of cross-linker, natural and synthetic polymers used in literature, mode of fabrication of hydrogels, and their different properties that are studied.…”

“… 29 Tuancharoensri et al engineered an SS/PHEMA hydrogel scaffold for tissue engineering, offering insights into tailoring hydrogel properties for potential use in skin tissue regeneration within tissue engineering contexts. 30 Critical literature review on the development of sericin-based hydrogels was conducted by different aspects such as type and nature of cross-linker, natural and synthetic polymers used in literature, mode of fabrication of hydrogels, and their different properties that are studied. To date, to our knowledge, PCL is novel for blending with sericin to study the controlled drug delivery system.…”