Effective tuning of ligand incorporation and mechanical properties in visible light photopolymerized poly(ethylene glycol) diacrylate hydrogels dictates cell adhesion and proliferation

Turturro, Michael V.; Sokic, Sonja; Larson, Jeffery C.; Papavasiliou, Georgia

doi:10.1088/1748-6041/8/2/025001

Cited by 33 publications

(31 citation statements)

References 40 publications

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“…Indeed, when NVP was added at 0.1 vol.% (9.36 mM; F2 in Table 1) or 1 vol.%, (93.6 mM; F3 in Table 1), the gel points were decreased from ~430 seconds to ~231 and ~92 seconds, respectively (Figure 2B, 2C, & Table 1). Increased gelation rate in the presence of NVP could be attributed to an increased vinyl group concentration and/or rapid diffusion of radical bearing NVP [10, 43]. …”

Section: Resultsmentioning

confidence: 99%

“…While NVP is a co-monomer that did not contribute to network cross-linking, adding NVP did increase the final gel stiffness. This is likely due to the formation of more hydrophobic and potentially more rigid poly(NVP) kinetic chains (Figure 1H) [10, 43]. Increasing NVP concentration also increased the likelihood of homopolymerization of multiple PEG-acrylate arms within the same cross-link.…”

Section: Resultsmentioning

confidence: 99%

“…It should be noted that the only function of TEOA in chain-growth gelation schemes is to provide radical species. An exceptionally high concentration (e.g., 225mM [30, 42, 43]) of TEOA was often used to generate sufficient radicals to initiate gelation. The use of high TEOA concentration may cause undesired cytotoxic effect to some sensitive cell types [40].…”

Section: Introductionmentioning

confidence: 99%

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Visible light cured thiol-vinyl hydrogels with tunable degradation for 3D cell culture

et al. 2014

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We report here a synthetically simple yet highly tunable and diverse visible light mediated thiol-vinyl gelation system for fabricating cell-instructive hydrogels. Gelation was achieved via a mixed-mode step-and-chain-growth photopolymerization using functionalized 4-arm poly(ethylene glycol) as backbone macromer, eosin-Y as photosensitizer, and di-thiol containing molecule as dual purpose co-initiator/cross-linker. N-vinylpyrrolidone (NVP) was used to accelerate gelation kinetics and to adjust the stiffness of the hydrogels. Visible light (wavelength: 400–700nm) was used to initiate rapid gelation (gel points: ~20 seconds) that reached completion within a few minutes. The major differences between current thiol-vinyl gelation and prior visible light mediated photopolymerization are that: (1) the co-initiator triethanolamine (TEOA) used in the previous systems was replaced with multifunctional thiols and (2) mixed-mode polymerized gels contain less network heterogeneity. The gelation kinetics and gel properties at the same PEG macromer concentration could be tuned by changing the identity of vinyl groups and di-thiol cross-linkers, as well as concentration of cross-linker and NVP. Specifically, acrylate-modified PEG afforded the fastest gelation rate, followed by acrylamide and methacrylate-functionalized PEG. Increasing NVP concentration also accelerated gelation and led to a higher network cross-linking density. Further, increasing di-thiol peptide concentration in the gel formulation increased hydrogel swelling and decreased gel stiffness. Due to the formation of thiol-ether-ester bonds following thiol-acrylate reaction, the gels degraded hydrolytically following a pseudo first order degradation kinetics. Degradation rate was controlled by adjusting thiol or NVP content in the polymer precursor solution. The cytocompatibility and utility of this hydrogel system were evaluated using in situ encapsulation of human mesenchymal stem cells (hMSC). Encapsulated hMSCs remained alive (>90%) throughout the duration of the study and the cells were differentiated down osteogenic lineage with varying degrees by controlling the rate and mode of gel degradation.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Visible light cured thiol-vinyl hydrogels with tunable degradation for 3D cell culture

et al. 2014

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“…The Illinois Institute of Technology chooses 15%, 25%, and 40% (w/v) PEGDA as the material to analyze cell adhesion and proliferation. The results show that increases in hydrogel concentration cause decreases in cell adhesion and increases in proliferation [19]. Therefore, 20% is a suitable concentration and can be adjusted if necessary for this study.…”

Section: Discussionmentioning

confidence: 98%

Development of a Robotic Arm Based Hydrogel Additive Manufacturing System for In-Situ Printing

Xiao

Lian

et al. 2017

Applied Sciences

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Abstract:In-situ printing is a promising injury repair technique that can be directly applied during surgical operations. This paper features a potential in-situ printing platform based on a small-scale robotic arm with a micro-sized dispenser valve. A double-light-source curing method was applied to print poly(ethylene glycol) diacrylate (PEGDA) with a 20% (weight/volume) ratio and the entire process was controlled automatically by a computer interface where droplet diameter, curing time, mechanical properties were measured and essential printing parameters (e.g., nozzle velocity, nozzle frequency) were determined. Three different two-dimensional (2D) plane models (namely, square, circular, and heart-shaped) were printed during initial printing trials. The feasibility study of in-situ printing on curved surfaces was tested using a three-dimensional (3D) printed defect model. The defect was successfully filled using both parallel and ring printing paths. In conclusion, the robotic arm printing platform and its forming method can achieve a rapid curing of PEGDA hydrogel on a curved surface and has the potential to be applied to in-situ printing.

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“…Having a PEG spacer, PEGDA hydrogels with RGD-MA can spread the cells specifically. Several cell lines such as chondrocytes, vascular endothelial cells (ECs), osteoblasts, neural cells, and marrow stromal cells (MSCs), and fibroblasts have been observed to immobilize on bioactive PEG hydrogels [37, 51, 66-68]. ACRL-PEG-RGD can copolymerize with PEGDA to create a cell-adhesive PEG second network in the IPN gels, but the distribution of RGD peptides in IPN hydrogels is assumed to be random because the RGD moiety is not expected to significantly affect the reactivity of the acrylate group and the extent of peptide incorporation in hydrogels is limited due to the monoacrylation of peptide, which affects hydrogel formation and its mechanical properties [50].…”

Section: Discussionmentioning

confidence: 99%

The bioactivity of agarose–PEGDA interpenetrating network hydrogels with covalently immobilized RGD peptides and physically entrapped aggrecan

2014

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Our previous reports of interpenetrating networks (IPNs) have demonstrated drastic improvements in mechanical performance relative to individual constituent networks while maintaining viability of encapsulated cells. The current study investigated whether covalent linkage of RGD to the poly(ethylene glycol) diacrylate (PEGDA) network could improve upon cell viability and performance of agarose-PEGDA IPNs compared to unmodified IPNs (control) and to IPNs with different concentrations of physically entrapped aggrecan, providing a point of comparison to previous work. The inclusion of RGD or aggrecan generally did not adversely affect mechanical performance, and significantly improved chondrocyte viability and performance. Although both 4 and 100 μ g/mL of aggrecan improved cell viability, only 100 μ g/mL aggrecan was clearly beneficial to improving biosynthesis, whereas 100 μg/mL of RGD was beneficial to both chondrocyte viability and biosynthesis. Interestingly, clustering of cells within the IPNs with RGD and the higher aggrecan concentration were observed, likely indicating cell migration and/or preferred regional proliferation. This clustering resulted in a clearly visible enhancement of matrix production compared to the other IPNs. With this cell migration, we also observed significant cell proliferation and matrix synthesis beyond the periphery of the IPN, which could have important implications in facilitating integration with surrounding cartilage in vivo. With RGD and aggrecan (at its higher concentration) providing substantial and comparable improvements in cell performance, RGD would be the recommended bioactive signal for this particular IPN formulation and cell source given the significant cost savings and potentially more straightforward regulatory pathway in commercialization.

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Effective tuning of ligand incorporation and mechanical properties in visible light photopolymerized poly(ethylene glycol) diacrylate hydrogels dictates cell adhesion and proliferation

Cited by 33 publications

References 40 publications

Visible light cured thiol-vinyl hydrogels with tunable degradation for 3D cell culture

Visible light cured thiol-vinyl hydrogels with tunable degradation for 3D cell culture

Development of a Robotic Arm Based Hydrogel Additive Manufacturing System for In-Situ Printing

The bioactivity of agarose–PEGDA interpenetrating network hydrogels with covalently immobilized RGD peptides and physically entrapped aggrecan

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