Flexible oligomer spacers as the key to solid-state photopolymerization of hydrogel precursors

Houben, Annemie; Roose, Patrice; Bergen, Hugues Van den; Declercq, Heidi; Hoorick, Jasper Van; Gruber, Peter; Ovsianikov, Aleksandr; Bontinck, Dirk; Vlierberghe, Sandra Van; Dubruel, Peter

doi:10.1016/j.mtchem.2017.01.005

Cited by 22 publications

(45 citation statements)

References 32 publications

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“… 46 , 47 This hypothesis is substantiated by the literature as similar observations were reported by Houben et al for synthetic cross-linkable hydrogel building blocks, where self-organization due to crystallization increased the observed cross-linking reactivity. 48 On the other hand, the formed triple helices are partially locked by the covalent cross-links thereby further increasing the final mechanical properties 46 , 47 (see Figure S3 ). As a consequence, UV-A irradiation of a physical network results in a more efficient cross-linking reaction, which is reflected by a substantially higher storage modulus obtained after cross-linking for both gel-MOD (i.e., 18 ± 1.3 vs 4.7 ± 0.3 kPa) and gel-MOD-AEMA (i.e., 60.6 ± 0.6 vs 14.9 ± 0.2 kPa) (comparison of Figure 3 A and B).…”

Section: Results and Discussionmentioning

confidence: 99%

Cross-Linkable Gelatins with Superior Mechanical Properties Through Carboxylic Acid Modification: Increasing the Two-Photon Polymerization Potential

et al. 2017

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The present work reports on the development of photo-cross-linkable gelatins sufficiently versatile to overcome current biopolymer two-photon polymerization (2PP) processing limitations. To this end, both the primary amines as well as the carboxylic acids of gelatin type B were functionalized with photo-cross-linkable moieties (up to 1 mmol/g) resulting in superior and tunable mechanical properties (G′ from 5000 to 147000 Pa) enabling efficient 2PP processing. The materials were characterized in depth prior to and after photoinduced cross-linking using fully functionalized gelatin-methacrylamide (gel-MOD) as a benchmark to assess the effect of functionalization on the protein properties, cross-linking efficiency, and mechanical properties. In addition, preliminary experiments on hydrogel films indicated excellent in vitro biocompatibility (close to 100% viability) both in the presence of MC3T3 preosteoblasts and L929 fibroblasts. Moreover, 2PP processing of the novel derivative was superior in terms of applied laser power (≥40 vs ≥60 mW for gel-MOD at 100 mm/s) as well as post-production swelling (0–20% vs 75–100% for gel-MOD) compared to those of gel-MOD. The reported novel gelatin derivative (gel-MOD-AEMA) proves to be extremely suitable for direct laser writing as both superior mimicry of the applied computer-aided design (CAD) was obtained while maintaining the desired cellular interactivity of the biopolymer. It can be anticipated that the present work will also be applicable to alternative biopolymers mimicking the extracellular environment such as collagen, elastin, and glycosaminoglycans, thereby expanding current material-related processing limitations in the tissue engineering field.

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Section: Results and Discussionmentioning

confidence: 99%

Cross-Linkable Gelatins with Superior Mechanical Properties Through Carboxylic Acid Modification: Increasing the Two-Photon Polymerization Potential

et al. 2017

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“…[ 29 ] These hydrogel precursors can be based on different polymer backbones, poly(ethylene glycol) (PEG) being one example only. [ 29,31–33 ] Cross‐linking in the solid state is promoted by the introduction of a flexible spacer which is linked to the backbone polymer by means of a di‐isocyanate (isophorone di‐isocyanate (IPDI)) (see Figure ). [ 29,31 ]…”

Section: Introductionmentioning

confidence: 99%

Activated Carbon Containing PEG‐Based Hydrogels as Novel Candidate Dressings for the Treatment of Malodorous Wounds

Minsart

Mignon

Arslan

et al. 2020

Macro Materials & Eng

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Malodorous wounds have a detrimental effect on the patient's well‐being. A dressing combining the properties of hydrogels and activated carbon (AC) would be beneficial for the treatment of these wounds, controlling wound exudate while adsorbing malodor‐causing compounds. The present work involves the use of acrylate‐endcapped, urethane‐based precursors (AUPs) and methacrylated alginate (AlgMOD). AUPs are synthesized with a varying poly(ethylene glycol) backbone molar mass (2–20 kg mol−1) to tune mechanical and swelling properties, whereas methacrylated alginate, known for its hemostatic properties, enables chemical cross‐linking. Blends of AUP and AlgMOD with AC are processed into hydrogel sheets and electrospun membranes. The results indicate tunable mechanical (Young's moduli 0.03–0.63 MPa) and swelling properties (2.2–34.9 gwater ) along with high gel fractions (>85%). The sheets are compared with commercial odor‐adsorbing dressings (Carbonet and Carboflex), enabling benchmarking. AUP sheets (8 and 10 kg mol−1) containing 0.5% w/w AC show strong adsorption (>90% after 24 h) of crystal violet. The obtained (core–shell AlgMOD/AUP) fibers are visualized using scanning and transmission electron microscopy. Indirect cell tests reveal the developed materials to be biocompatible. In conclusion, a hydrogel‐based odor‐adsorbing wound dressing is successfully synthesized and holds promise for malodorous wound healing.

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“…By varying the concentration, the final material properties can be tailored depending on the envisaged application. In addition, the material can be crosslinked efficiently in the absence of a photoinitiator, avoiding preprocessing mixing steps and potential toxic effects of the photoinitiator . To select the most appropriate hydrogel concentration for the scaffold fabrication, rheology, tensile, and swelling tests were conducted.…”

Section: Resultsmentioning

confidence: 99%

“…An acrylate‐endcapped urethane‐based poly(ethylene glycol) (AUP) was synthesized by reacting poly(ethylene glycol) ( M n 2000 g mol −1 ) (PEG 2000, Sigma) with isophorone diisocyanate (IPDI, BASF) at 75 °C in a 1:2 stoichiometric ratio, using 300 ppm of bismuth neodecanoate (Shepherd) as a catalyst. Next, a monoacrylated PEG (Bisomer PEA 6, GEO Specialty Chemicals UK Ltd.) was added together with 300 ppm of bismuth neodecanoate and the temperature was held at 80 °C until the reaction was completed.…”

Section: Methodsmentioning

confidence: 99%

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Indirect Solid Freeform Fabrication of an Initiator‐Free Photocrosslinkable Hydrogel Precursor for the Creation of Porous Scaffolds

Houben

Pien

et al. 2016

Macromolecular Bioscience

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In the present work, a photopolymerized urethane-based poly(ethylene glycol) hydrogel is applied as a porous scaffold material using indirect solid freeform fabrication (SFF). This approach combines the benefits of SFF with a large freedom in material selection and applicable concentration ranges. A sacrificial 3D poly(ε-caprolactone) structure is generated using fused deposition modeling and used as template to produce hydrogel scaffolds. By changing the template plotting parameters, the scaffold channel sizes vary from 280 to 360 μm, and the strut diameters from 340 to 400 μm. This enables the production of scaffolds with tunable mechanical properties, characterized by an average hardness ranging from 9 to 43 N and from 1 to 6 N for dry and hydrated scaffolds, respectively. Experiments using mouse calvaria preosteoblasts indicate that a gelatin methacrylamide coating of the scaffolds results in an increased cell adhesion and proliferation with improved cell morphology.

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Flexible oligomer spacers as the key to solid-state photopolymerization of hydrogel precursors

Cited by 22 publications

References 32 publications

Cross-Linkable Gelatins with Superior Mechanical Properties Through Carboxylic Acid Modification: Increasing the Two-Photon Polymerization Potential

Cross-Linkable Gelatins with Superior Mechanical Properties Through Carboxylic Acid Modification: Increasing the Two-Photon Polymerization Potential

Activated Carbon Containing PEG‐Based Hydrogels as Novel Candidate Dressings for the Treatment of Malodorous Wounds

Indirect Solid Freeform Fabrication of an Initiator‐Free Photocrosslinkable Hydrogel Precursor for the Creation of Porous Scaffolds

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