A thermo-responsive and photo-polymerizable chondroitin sulfate-based hydrogel for 3D printing applications

Abbadessa, Anna; Blokzijl, Maarten M.; Mouser, Vivian H. M.; Marica, P.; Malda, Jos; Hennink, Wim E.; Vermonden, Tina

doi:10.1016/j.carbpol.2016.04.080

Cited by 119 publications

(104 citation statements)

References 53 publications

(69 reference statements)

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“…HA and HAMA were characterized by GPC [23]. HAMA was analyzed by 1 in which an integration value of 1 is given to the signal at chemical shift of 6.2 ppm.…”

Section: Synthesis and Characterization Of Polymersmentioning

confidence: 99%

“…Specifically, the more pronounced thermosensitivity, shear thinning and yield stress behavior led to a superior 3D printability of hydrogels based on polysaccharides and PEG/methacrylated pHPMAlac copolymers compared with hydrogels only composed of PEG/methacrylated pHPMAlac copolymers [23,24]. Nevertheless, mechanistic insights behind the beneficial effect on mechanical properties due to the addition of polysaccharides to hydrogels of PEG/methacrylated pHPMAlac are lacking.…”

Section: Introductionmentioning

confidence: 97%

“…Nevertheless, mechanistic insights behind the beneficial effect on mechanical properties due to the addition of polysaccharides to hydrogels of PEG/methacrylated pHPMAlac are lacking. Visual inspection of these hydrogels pointed to the possibility of aqueous two phase separation (ATPS) [23], similar to that described for some pairs of water soluble polymers, such as the combination of PEG and dextran [25]. The miscibility of two polymers in water is governed by the following equation:…”

Section: Introductionmentioning

confidence: 97%

“…Our more recent studies have shown that by blending these PEG/methacrylated pHPMAlac triblock copolymers with UV cross-linkable polysaccharides, i.e. methacrylated chondroitin sulfate [23] or methacrylated hyaluronic acid [24], hydrogels with improved mechanical characteristics and degradation profiles can be obtained.…”

Section: Introductionmentioning

confidence: 98%

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Two-component thermosensitive hydrogels: Phase separation affecting rheological behavior

Abbadessa

Landín

Blenke

et al. 2017

European Polymer Journal

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Please cite this article as: Abbadessa, A., Landín, M., Oude Blenke, E., Hennink, W.E., Vermonden, T., Twocomponent thermosensitive hydrogels: Phase separation affecting rheological behavior, European Polymer Journal (2017), doi: http://dx. AbstractExtracellular matrices are mainly composed of a mixture of different biopolymers and therefore the use of two or more building blocks for the development of tissue-mimicking hydrogels is nowadays an attractive strategy in tissue-engineering. Multi-component hydrogel systems may undergo phase separation, which in turn can lead to new, unexpected material properties. The aim of this study was to understand the role of phase separation on the mechanical properties and 3D printability of hydrogels composed of triblock copolymers of polyethylene glycol (PEG) and methacrylated poly(N-(2-hydroxypropyl) methacrylamide-mono/dilactate) (pHPMAlac) blended with methacrylated hyaluronic acid (HAMA). To this end, hydrogels composed of different concentrations of PEG/pHPMAlac and HAMA, were analyzed for phase behavior and rheologicalproperties. Subsequently, phase separation and rheological behavior as function of the two polymer concentrations were mathematically processed to generate a predictive model. Results showed that PEG/pHPMAlac/HAMA hydrogels were characterized by hydrophilic, HAMA-richer internal domains dispersed in a more hydrophobic continuous phase, composed of PEG/pHPMAlac, and that the volume fraction of the dispersed phase increased by increasing HAMA concentration.Storage modulus, yield stress and viscosity increased with increasing HAMA concentration for low/medium HAMA contents (• 0.75% w/w), while a further increase of HAMA resulted in a 0.75% w/w), while a further increase of HAMA resulted in a decrease of the mentioned properties. On the other hand, by increasing the concentration of PEG/pHPMAlac these rheological properties were enhanced. The generated models showed a good fitting with experimental data, and were used to identify an exemplary 3D printability window for PEG/pHPMAlac/HAMA hydrogels, which was verified by rheological characterization and preparation of 3D printed scaffolds. In conclusion, a clear relationship between phase separation and rheological behavior in these two-component hydrogels can be described by complex functions of the two polymer concentrations. The predictive model generated in this study can be used as a valid tool for the identification of hydrogel compositions with desired, selected characteristics.3 Keywords: Thermosensitive polymers, hyaluronic acid, rheological properties, confocal laser scanning microscopy, neurofuzzy logic, 3D bioprinting. Highlights-Polymer ratios determine extent of phase separation in PEG/pHPMAlac/HAMA hydrogels.-Phase separation leads to hydrophilic domains dispersed in a more hydrophobic phase.-Phase separation affects rheological properties in a controllable fashion.-Mathematical models enabled a priori identification of hydrogels with desired properties.-Hydrogel 3D printing was achieved with a f...

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“…HA and HAMA were characterized by GPC [23]. HAMA was analyzed by 1 in which an integration value of 1 is given to the signal at chemical shift of 6.2 ppm.…”

Section: Synthesis and Characterization Of Polymersmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 97%

Section: Introductionmentioning

confidence: 97%

Section: Introductionmentioning

confidence: 98%

See 2 more Smart Citations

Two-component thermosensitive hydrogels: Phase separation affecting rheological behavior

Abbadessa

Landín

Blenke

et al. 2017

European Polymer Journal

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show abstract

“…The results obtained from the µCT were in agreement with previous studies where no horizontal pores interconnectivity was found for a 3D printable UV photocrosslinkable methacrylated chondroitin sulphated-based scaffolds combined with a thermosensitive triblock copolymer with a G' around 380 Pa at 40 °C [53]. Extrudable hydrogel-based inks with high water content typically display collapse of the single filament leading to a unidirectional porosity along the top view of the scaffold, and transversal porosity preservation remains an unmet challenge.…”

Section: Discussionsupporting

confidence: 81%

Development of hyaluronic acid derivatives for applications in biomedical engineering

Petta¹

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Engineered Hydrogels

Bektas¹,

Usal²,

Hasırcı³

et al. 2021

Biological Soft Matter

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A thermo-responsive and photo-polymerizable chondroitin sulfate-based hydrogel for 3D printing applications

Cited by 119 publications

References 53 publications

Two-component thermosensitive hydrogels: Phase separation affecting rheological behavior

Two-component thermosensitive hydrogels: Phase separation affecting rheological behavior

Development of hyaluronic acid derivatives for applications in biomedical engineering

Engineered Hydrogels

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