Interpenetrating network design of bioactive hydrogel coatings with enhanced damage resistance

Wancura, Megan; Nkansah, Abbey; Chwatko, Malgorzata; Robinson, Andrew; Fairley, Ashauntee; Cosgriff‐Hernandez, Elizabeth

doi:10.1039/d2tb02825e

Cited by 11 publications

(19 citation statements)

References 107 publications

(197 reference statements)

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“…Polyether urethane diacrylamide (PEUDAm) was synthetized as previously described. 33 Diffusion-mediated redox crosslinking was performed to hydrogel coat the electrospun polyurethane meshes. 23,33 Briefly, mesh substrates (0.18-0.24 mm thick) were cut to 1.2 x 1.2 cm squares or 2.2 x 2.2 cm squares and soaked in a wetting ladder of decreasing concentrations of ethanol (70 vol%, 50 vol%, 30 vol%, and 0 vol% ethanol in water, 15 minutes each).…”

Section: Methodsmentioning

confidence: 99%

“…33 Diffusion-mediated redox crosslinking was performed to hydrogel coat the electrospun polyurethane meshes. 23,33 Briefly, mesh substrates (0.18-0.24 mm thick) were cut to 1.2 x 1.2 cm squares or 2.2 x 2.2 cm squares and soaked in a wetting ladder of decreasing concentrations of ethanol (70 vol%, 50 vol%, 30 vol%, and 0 vol% ethanol in water, 15 minutes each). Iron gluconate was then adsorped onto the substrates by immersing the meshes in iron gluconate dihydrate solutions (IG, 3 wt/vol% [Fe 2+ ], as determined with the Ferrozine Assay 37 ) for 15 minutes.…”

Section: Methodsmentioning

confidence: 99%

“…For improved toughness, a second interpenetrating network was incorporated based on our previous report. 33 The dried composites were swollen in a solution of 20 wt/vol% N- acryloyl glycinamide (NAGA; BLD Pharma), 0.1 mol% bisacrylamide (bisAAm), and 2 wt/vol% Irgacure 2959 overnight protected from light at 4 °C. Swollen substrates were placed on a glass plate and cured for 20 minutes on each side via photopolymerization under a UV transilluminator (Intelligent Ray Shuttered UV Flood Light, Integrated Dispensing Solutions, Inc., 365 nm, 4 mW/cm 2 ).…”

Section: Methodsmentioning

confidence: 99%

“…As an initial assessment of thromboresistance, static platelet attachment was characterized as previously described in literature. 33,41 Glutaraldehyde-fixed pericardium and hydrogel-polyurethane fiber composites were prepared by immersion in 70% ethanol for 3 hours. Samples were then subjected to a wetting ladder with sequential soaks in 50%, 30% and 0% ethanol in PBS for 30 min each.…”

Section: Methodsmentioning

confidence: 99%

“…A custom 3D printed setup consisting of a chamber and hanger was then developed to apply unform coatings to device-level electrospun tubes using our redox-based coating platform. 33 The hydrogel-polyurethane fiber composite tubes were sutured to a cobalt chromium stent for device level testing of hemodynamics. To enhance long-term durability, electrospinning methodology was developed to improve control of fiber alignment, curvilinear alignment, and tortuous microarchitectures.…”

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confidence: 99%

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Hydrogel-polyurethane fiber composites with enhanced microarchitectural control for heart valve replacement

Robinson,

Nkansah,

Bhat

et al. 2023

Preprint

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Polymeric heart valves offer the potential to overcome the limited durability of tissue based bioprosthetic valves and the need for anticoagulant therapy of mechanical valve replacement options. However, developing a single-phase material with requisite biological properties and target mechanical properties remains a challenge. In this study, a composite heart valve material was developed where an electrospun mesh provides tunable mechanical properties and a hydrogel coating confers an antifouling surface for thromboresistance. Key biological responses were evaluated in comparison to glutaraldehyde-fixed pericardium. Platelet and bacterial attachment were reduced by 38% and 98%, respectively, as compared to pericardium that demonstrated the antifouling nature of the hydrogel coating. There was also a notable reduction (59%) in the calcification of the composite material as compared to pericardium. A custom 3D printed hydrogel coating setup was developed to make valve composites for device-level hemodynamic testing. Regurgitation fraction (9.6 ± 1.8%) and effective orifice area (1.52 ± 0.34 cm2) met ISO 5840-2:2021 requirements. Additionally, the mean pressure gradient was comparable to current clinical bioprosthetic heart valves demonstrating preliminary efficacy. Although the hemodynamic properties are promising, it is anticipated that the random microarchitecture will result in suboptimal strain fields and peak stresses that may accelerate leaflet fatigue and degeneration. Previous computational work has demonstrated that bioinspired fiber microarchitectures can improve strain homogeneity of valve materials toward improving durability. To this end, we developed advanced electrospinning methodologies to achieve polyurethane fiber microarchitectures that mimic or exceed the physiological ranges of alignment, tortuosity, and curvilinearity present in the native valve. Control of fiber alignment from a random fiber orientation at a normalized orientation index (NOI) 14.2 ± 6.9% to highly aligned fibers at a NOI of 85.1 ± 1.4%. was achieved through increasing mandrel rotational velocity. Fiber tortuosity and curvilinearity in the range of native valve features were introduced through a post-spinning annealing process and fiber collection on a conical mandrel geometry, respectively. Overall, these studies demonstrate the potential of hydrogel-polyurethane fiber composite as a heart valve material. Future studies will utilize the developed advanced electrospinning methodologies in combination with model-directed fabrication toward optimizing durability as a function of fiber microarchitecture.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

mentioning

confidence: 99%

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Hydrogel-polyurethane fiber composites with enhanced microarchitectural control for heart valve replacement

Robinson,

Nkansah,

Bhat

et al. 2023

Preprint

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A user's guide to degradation testing of polyethylene glycol‐based hydrogels: From in vitro to in vivo studies

Rodriguez‐Rivera,

Green,

Shah

et al. 2023

J Biomedical Materials Res

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Poly(ethylene glycol) (PEG)‐based hydrogels have gained significant attention in the field of biomedical applications due to their versatility and antifouling properties. Acrylate‐derivatized PEG hydrogels (PEGDA) are some of the most widely studied hydrogels; however, there has been debate around the degradation mechanism and predicting resorption rates. Several factors influence the degradation rate of PEG hydrogels, including backbone and endgroup chemistry, macromer molecular weight, and polymer concentration. In addition to hydrogel parameters, it is necessary to understand the influence of biological and environmental conditions (e.g., pH and temperature) on hydrogel degradation. Rigorous methods for monitoring degradation in both in vitro and in vivo settings are also critical to hydrogel design and development. Herein, we provide guidance on tailoring PEG hydrogel chemistry to achieve target hydrolytic degradation kinetics for both resorbable and biostable applications. A detailed overview of accelerated testing methods and hydrogel degradation characterization is provided to aid researchers in experimental design and interpreting in vitro–in vivo correlations necessary for predicting hydrogel device performance.

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Hydrogel‐polyurethane fiber composites with enhanced microarchitectural control for heart valve replacement

Robinson,

Nkansah,

Bhat

et al. 2023

J Biomedical Materials Res

Self Cite

View full text Add to dashboard Cite

Polymeric heart valves offer the potential to overcome the limited durability of tissue based bioprosthetic valves and the need for anticoagulant therapy of mechanical valve replacement options. However, developing a single‐phase material with requisite biological properties and target mechanical properties remains a challenge. In this study, a composite heart valve material was developed where an electrospun mesh provides tunable mechanical properties and a hydrogel coating confers an antifouling surface for thromboresistance. Key biological responses were evaluated in comparison to glutaraldehyde‐fixed pericardium. Platelet and bacterial attachment were reduced by 38% and 98%, respectively, as compared to pericardium that demonstrated the antifouling nature of the hydrogel coating. There was also a notable reduction (59%) in the calcification of the composite material as compared to pericardium. A custom 3D‐printed hydrogel coating setup was developed to make valve composites for device‐level hemodynamic testing. Regurgitation fraction (9.6 ± 1.8%) and effective orifice area (1.52 ± 0.34 cm2) met ISO 5840‐2:2021 requirements. Additionally, the mean pressure gradient was comparable to current clinical bioprosthetic heart valves demonstrating preliminary efficacy. Although the hemodynamic properties are promising, it is anticipated that the random microarchitecture will result in suboptimal strain fields and peak stresses that may accelerate leaflet fatigue and degeneration. Previous computational work has demonstrated that bioinspired fiber microarchitectures can improve strain homogeneity of valve materials toward improving durability. To this end, we developed advanced electrospinning methodologies to achieve polyurethane fiber microarchitectures that mimic or exceed the physiological ranges of alignment, tortuosity, and curvilinearity present in the native valve. Control of fiber alignment from a random fiber orientation at a normalized orientation index (NOI) 14.2 ± 6.9% to highly aligned fibers at a NOI of 85.1 ± 1.4%. was achieved through increasing mandrel rotational velocity. Fiber tortuosity and curvilinearity in the range of native valve features were introduced through a post‐spinning annealing process and fiber collection on a conical mandrel geometry, respectively. Overall, these studies demonstrate the potential of hydrogel‐polyurethane fiber composite as a heart valve material. Future studies will utilize the developed advanced electrospinning methodologies in combination with model‐directed fabrication toward optimizing durability as a function of fiber microarchitecture.

show abstract

Interpenetrating network design of bioactive hydrogel coatings with enhanced damage resistance

Abstract: Bioactive hydrogel coatings offer a promising route to introduce sustained thromboresistance to cardiovascular devices without compromising bulk mechanical properties. Poly(ethylene glycol)-based hydrogels provide antifouling properties to limit acute thromobosis and...

Cited by 11 publications

References 107 publications

Hydrogel-polyurethane fiber composites with enhanced microarchitectural control for heart valve replacement

Hydrogel-polyurethane fiber composites with enhanced microarchitectural control for heart valve replacement

A user's guide to degradation testing of polyethylene glycol‐based hydrogels: From in vitro to in vivo studies

Hydrogel‐polyurethane fiber composites with enhanced microarchitectural control for heart valve replacement

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