Dataset Information

Rate-Dependent Stiffness and Recovery in Interpenetrating Network Hydrogels through Sacrificial Metal Coordination Bonds.

ABSTRACT: Four-arm poly(ethylene glycol) (PEG) star polymers modified with 3-hydroxy-4-pyridinone (HOPO) end groups were shown to form transient, coordination networks upon addition of trivalent cations In3+, Fe3+, and Al3+. These coordination-based hydrogels exhibited high activation energies of viscoelasticity (34 kT) and characteristic bond lifetimes tunable over 2 orders of magnitude and could be incorporated into poly(hydroxyethylacrylamide)-based covalent scaffolds to create interpenetrating network hydrogels. Measurements carried out in compression and tension demonstrate that the secondary coordination network imparts toughness and stiffness to the overall material, and unlike traditional interpenetrating networks (IPNs), the extent of toughening is dependent on the rate at which the materials are deformed. The dynamic character of the coordination network also allows recovery after mechanical damage following high amplitude strains.

SUBMITTER: Menyo MS

PROVIDER: S-EPMC5096649 | biostudies-literature | 2015 Nov

REPOSITORIES: biostudies-literature

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Rate-Dependent Stiffness and Recovery in Interpenetrating Network Hydrogels through Sacrificial Metal Coordination Bonds.

Menyo Matthew S MS Hawker Craig J CJ Waite J Herbert JH

ACS macro letters 20151015 11

Four-arm poly(ethylene glycol) (PEG) star polymers modified with 3-hydroxy-4-pyridinone (HOPO) end groups were shown to form transient, coordination networks upon addition of trivalent cations In3+, Fe3+, and Al3+. These coordination-based hydrogels exhibited high activation energies of viscoelasticity (34 kT) and characteristic bond lifetimes tunable over 2 orders of magnitude and could be incorporated into poly(hydroxyethylacrylamide)-based covalent scaffolds t ...[more]

PMID: 27818845

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Project description:Hydrogels are effective platforms for use as artificial extracellular matrices, cell carriers, and to present bioactive cues. Two common natural polymers, fibrin and alginate, are broadly used to form hydrogels and have numerous advantages over synthetic materials. Fibrin is a provisional matrix containing native adhesion motifs for cell engagement, yet the interplay between mechanical properties, degradation, and gelation rate is difficult to decouple. Conversely, alginate is highly tunable yet bioinert and requires modification to present necessary adhesion ligands. To address these challenges, we developed a fibrin-alginate interpenetrating network (IPN) hydrogel to combine the desirable adhesion and stimulatory characteristics of fibrin with the tunable mechanical properties of alginate. We tested its efficacy by examining capillary network formation with entrapped co-cultures of mesenchymal stromal cells (MSCs) and endothelial cells (ECs). We manipulated thrombin concentration and alginate crosslinking density independently to modulate the fibrin structure, mesh size, degradation, and biomechanical properties of these constructs. In IPNs of lower stiffness, we observed a significant increase in total cell area (1.7 × 105 ± 7.9 × 104 µm2) and decrease in circularity (0.56 ± 0.03) compared to cells encapsulated in stiffer IPNs (4.0 × 104 ± 1.5 × 104 µm2 and 0.77 ± 0.09, respectively). Fibrinogen content did not influence capillary network formation. However, higher fibrinogen content led to greater retention of these networks confirmed via increased spreading and presence of F-actin at 7 days. This is an elegant platform to decouple cell adhesion and hydrogel bulk stiffness that will be broadly useful for cell instruction and delivery. STATEMENT OF SIGNIFICANCE: Hydrogels are widely used as drug and cell delivery vehicles and as artificial extracellular matrices to study cellular responses. However, there are limited opportunities to simultaneously control mechanical properties and degradation while mimicking the complex native adhesion motifs and ligands known to encourage cell engagement with the hydrogel. In this study, we describe a fibrin-alginate interpenetrating network (IPN) hydrogel designed to balance the compliance and provisional qualities of fibrin with the mechanical stability and tunability of alginate to interrogate these contributions on cell response. We used clinically relevant cell sources, a co-culture of endothelial cells and mesenchymal stromal cells, to test its efficacy in supporting capillary formation in vitro. These data demonstrate the promise of this IPN for use in tissue engineering.

Project description:Small-caliber vascular grafts used in coronary artery bypass procedures typically fail due to the development of intimal hyperplasia or thrombosis. Our laboratory has developed a multilayered vascular graft with an electrospun polyurethane outer layer with improved compliance matching and a hydrogel inner layer that is both thromboresistant and promotes endothelialization. Initial in vivo studies showed that hydrogel particulates were dislodged from the hydrogel layer of the grafts during suturing. To address this problem, we developed and characterized a new hydrogel formulation that resists damage during suturing. Introduction of sacrificial, hydrogen bonds to poly(ethylene glycol)-based hydrogels via co-polymerization with n-vinyl pyrrolidone (NVP) increased the fracture energy as determined by single edge notch testing. This enhanced defect tolerance resulted in a hydrogel layer that was resistant to suture-induced damage with no dislodged particles observed. Importantly, the incorporation of NVP did not affect the thromboresistance, bioactivity, or biostability of the hydrogel layer. In addition to eliminating complications due to hydrogel particle generation in our multilayer graft design, this defect tolerant hydrogel formulation has broad potential use in many cardiovascular and soft tissue applications. STATEMENT OF SIGNIFICANCE:Small-caliber vascular grafts used in coronary artery bypass procedures typically fail due to development of intimal hyperplasia or thrombosis. Our laboratory has developed a multilayered vascular graft with an electrospun polyurethane outer layer with improved compliance matching and a hydrogel inner layer that is both thromboresistant and promotes endothelialization. However, hydrogel particulates were dislodged from the hydrogel layer during suturing in vivo. This work describes a hydrogel formulation based on poly(ethylene glycol) that is resistant to suture-induced damage. The introduction of sacrificial, hydrogen bonds by co-polymerization with n-vinyl pyrrolidone (NVP) resulted in an increase fracture energy without affecting the thromboresistance, bioactivity, or biostability. This defect-tolerant hydrogel formulation and the methodology to assess hydrogel defect tolerance has broad potential use in cardiovascular and soft tissue applications.

Dataset Information

Rate-Dependent Stiffness and Recovery in Interpenetrating Network Hydrogels through Sacrificial Metal Coordination Bonds.

Publications

Rate-Dependent Stiffness and Recovery in Interpenetrating Network Hydrogels through Sacrificial Metal Coordination Bonds.

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