2022
DOI: 10.1021/acsomega.2c03031
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Tailoring Physical Properties of Dual-Network Acrylamide Hydrogel Composites by Engineering Molecular Structures of the Cross-linked Network

Abstract: We demonstrate the impact of engineering molecular structures of poly(acrylamide) (PAAm) and poly( N -isopropylacrylamide) (PNIPAm) hydrogel composites on several physical properties. The network structure was systematically varied by (i) the type and the concentration of difunctional cross-linkers and (ii) the type of native or chemically modified natural polymers, including sodium alginate, methacrylate/dopamine-incorporated porcine skin gelatin and fish skin gelatin, and thiol-incorpo… Show more

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Cited by 6 publications
(4 citation statements)
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“…fGel was selected because of its straightforward anchoring points for cell attachment, its chemical versatility to incorporate reactive groups, and its abundance and sustainability. , However, the primary amine of lysine in the fGel can react with DTC or glycidyl groups, making it challenging to prepare the composite thin film from the coating solution. To overcome this issue, we modified fGel to incorporate methacrylate units, which can act as crosslinkable units in the presence of a radical species, by reacting the primary amine with the glycidyl group in glycidyl methacrylate, i.e., fGelMA. ,, In this design, two crosslinking mechanisms are considered after UV light illumination: (i) addition of the released primary amine from NBOC in MN with DTC or glycidyl groups in the MD or MG chain and (ii) a radical-based reaction of the methacrylate in fGelMA (Scheme ) with the use of a photo-radical generator (LAP). In the case of the MN/MG system, the vinyl groups in the fGelMA chains were bonded to each other to form interchain bridges upon exposure, with the resulting fGelMA network expected to be intertwined and physically interact with another network formed by interchain reactions between the MN and MG chains.…”
Section: Resultsmentioning
confidence: 99%
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“…fGel was selected because of its straightforward anchoring points for cell attachment, its chemical versatility to incorporate reactive groups, and its abundance and sustainability. , However, the primary amine of lysine in the fGel can react with DTC or glycidyl groups, making it challenging to prepare the composite thin film from the coating solution. To overcome this issue, we modified fGel to incorporate methacrylate units, which can act as crosslinkable units in the presence of a radical species, by reacting the primary amine with the glycidyl group in glycidyl methacrylate, i.e., fGelMA. ,, In this design, two crosslinking mechanisms are considered after UV light illumination: (i) addition of the released primary amine from NBOC in MN with DTC or glycidyl groups in the MD or MG chain and (ii) a radical-based reaction of the methacrylate in fGelMA (Scheme ) with the use of a photo-radical generator (LAP). In the case of the MN/MG system, the vinyl groups in the fGelMA chains were bonded to each other to form interchain bridges upon exposure, with the resulting fGelMA network expected to be intertwined and physically interact with another network formed by interchain reactions between the MN and MG chains.…”
Section: Resultsmentioning
confidence: 99%
“…Furthermore, due to the presence of highly polar PEG units in all copolymers, dual-component systems consisting of MN and MG or MN and MD were all processable with polar solvents, e.g., water and ethanol, and readily crosslinked simply by UV light illumination, which allows defining and stabilizing an active thin film surface in a desirable region by a photolithographic manner, without any additives and heating process. We further utilized the designed materials and resulting surfaces to attain surface activeness by incorporating biologically active macromolecules via two routes: (i) the resulting thin films were further modified with the reaction of bovine serum albumin (BSA) in the presence of the remaining surface reactive groups (epoxide and DTC); (ii) the copolymers were further mixed with fish skin gelatin bearing methacrylate , to form the composite thin film, further allowing additional crosslinking in the presence of a photo-radical generator. The amount of gelatin imparting surface-active functionality was also controllable without any degradation in the crosslinking capability.…”
Section: Introductionmentioning
confidence: 99%
“…18 On the basis of the relatively low solubilities (CaO 2 1.65 mg/mL at 20 °C and MgO 2 0.86 mg/ mL at 18 °C19 ), calcium peroxide has a higher oxygengeneration potential than magnesium peroxide. 20 Therefore, to apply antioxidation and locoregional oxygenation, we developed injectable lignin composites with the following components and properties: (1) lignosulfonate with thiolation (TLS) that scavenges ROS from wounds, 21,22 (2) unmodified sodium lignosulfonate (SLS) that encapsulates CaO 2 while scavenging radicals from CaO 2 15,23 and simultaneously protecting CaO 2 from an aqueous environment of tissue or hydrogel, and (3) methacrylated gelatin (GelMA) that modulates the mechanical properties 22 of lignin composites to support injectability. The first two rationales can confer the dual functionality of lignosulfonate.…”
Section: Introductionmentioning
confidence: 99%
“…Therefore, to apply antioxidation and locoregional oxygenation, we developed injectable lignin composites with the following components and properties: 1) thiolated lignosulfonate (TLS) scavenges ROS from wounds[33, 34], 2) methacrylated gelatin (GelMA) modulates the mechanical properties[34] of lignin composites to support injectability, and 3) sodium lignosulfonate (SLS)[26] encapsulates CaO 2 while scavenging radicals from CaO 2 [26, 35] and simultaneously protecting CaO 2 from aqueous environment of tissue or hydrogel. First, we assessed the integration of CaO 2 to SLS-PLGA (poly(lactic- co -glycolic) acid) nanoparticles (NPs) and the release of O 2 from lignin composites.…”
Section: Introductionmentioning
confidence: 99%