Development of Polyhydroxyalkanoate-Based Polyurethane with Water-Thermal Response Shape-Memory Behavior as New 3D Elastomers Scaffolds.
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ABSTRACT:
SUBMITTER: Wang C
PROVIDER: S-EPMC6631955 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Patients with bone defects suffer from a high rate of disability and deformity. Poor contact of grafts with defective bones and insufficient osteogenic activities lead to increased loose risks and unsatisfied repair efficacy. Although self-expanding scaffolds were developed to enhance bone integration, the limitations on the high transition temperature and the unsatisfied bioactivity hindered greatly their clinical application. Herein, we report a near-infrared-responsive and tight-contacting scaffold that comprises of shape memory polyurethane (SMPU) as the thermal-responsive matrix and magnesium (Mg) as the photothermal and bioactive component, which fabricated by the low temperature rapid prototyping (LT-RP) 3D printing technology. As designed, due to synergistic effects of the components and the fabrication approach, the composite scaffold possesses a homogeneously porous structure, significantly improved mechanical properties and stable photothermal effects. The programmed scaffold can be heated to recover under near infrared irradiation in 60s. With 4 wt% Mg, the scaffold has the balanced shape fixity ratio of 93.6% and shape recovery ratio of 95.4%. The compressed composite scaffold could lift a 100 g weight under NIR light, which was more than 1700 times of its own weight. The results of the push-out tests and the finite element analysis (FEA) confirmed the tight-contacting ability of the SMPU/4 wt%Mg scaffold, which had a signficant enhancement compared to the scaffold without shape memory effects. Furthermore, The osteopromotive function of the scaffold has been demonstrated through a series of in vitro and in vivo studies. We envision this scaffold can be a clinically effective strategy for robust bone regeneration.
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Project description:Water-blown polyurethane (PU) foams are of enormous technological interest as they are widely applied in various fields, i.e., consumer goods, medicine, automotive or aerospace industries. The discovery of the one-way shape-memory effect in PU foams provided a fresh impetus for extensive investigations on porous polymeric actuators over the past decades. High expansion ratios during the shape-recovery are of special interest when big volume changes are required, for example to fill an aneurysm during micro-invasive surgery or save space during transportation. However, the need to program the foams before each operation cycle could be a drawback impeding the entry of shape-memory polymeric (SMP) foams to our daily life. Here, we showed that a reversible shape-memory effect (rSME) is achievable for polyurethane water-blown semicrystalline foams. We selected commercially available crystallizable poly(ε-caprolactone)-diols of different molecular weight for foams synthesis, followed by investigations of morphology, thermal, thermomechanical and shape-memory properties of obtained compositions. Densities of synthesized foams varied from 110 to 180 kg∙m-3, while peak melting temperatures were composition-dependent and changed from 36 to 47 °C, while the melting temperature interval was around 15 K. All semicrystalline foams exhibited excellent one-way SME with shape-fixity ratios slightly above 100% and shape-recovery ratios from the second cycle of 99%. The composition with broad distribution of molecular weights of poly(ε-caprolactone)-diols exhibited an rSME of about 12% upon cyclic heating and cooling from Tlow = 10 °C and Thigh = 47 °C. We anticipate that our experimental study opens a field of systematic investigation of rSMEs in porous polymeric materials on macro and micro scale and extend the application of water-blown polyurethane foams to, e.g., protective covers with zero thermal expansion or even cushions adjustable to a certain body shape.
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Project description:Shape-memory polymers tend to present rigid behavior at ambient temperature, being unable to deform in this state. To obtain soft shape-memory elastomers, composites based on a commercial rubber crosslinked by both ionic and covalent bonds were developed, as these materials do not lose their elastomeric behavior below their transition (or activation) temperature (using ionic transition for such a purpose). The introduction of fillers, such as carbon black and multiwalled carbon nanotubes (MWCNTs), was studied and compared with the unfilled matrix. By adding contents above 10 phr of MWCNT, shape-memory properties were enhanced by 10%, achieving fixing and recovery ratios above 90% and a faster response. Moreover, by adding these fillers, the conductivity of the materials increased from ~10-11 to ~10-4 S·cm-1, allowing the possibility to activate the shape-memory effect with an electric current, based on the heating of the material by the Joule effect, achieving a fast and clean stimulus requiring only a current source of 50 V.
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Project description:Shape-memory composites have benefits for minimally invasive surgery, but their wider applications for bone repair are hindered by conflicts between the mechanical and memory performances, especially at load-bearing locations. In this study, we fabricated a graphene oxide shape-memory polyurethane composite through the chemical combination of graphene oxide and isocyanate, in order to realize satisfactory mechanical and shape-memory effects. As desired, a modulus of ~339 MPa and a shape recovery ratio of 98% were achieved, respectively, in the composite. In addition, finite element analysis demonstrated that, after being implanted in a defective bone through a minimally invasive treatment, where the highest stress was distributed at the implant-bone interface, this composite could offer a generated force during the recovery process. Furthermore, we also discuss the origins of the improved mechanical and memory properties of the composites, which arise from increased net-points and the stable molecular structure inside. Therefore, with its superior structure and properties, we envision that this shape-memory composite can provide new insights toward the practical application of shape-memory polymers and composites in the field of bone repair.
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Project description:In this work, small molecule diols named PEMTC were synthesized from isophorone diisocyanate, N-(2-hydroxyethyl)acrylamide and trimethylolpropane by a semi-directional method. PEMTC (2-(prop-2-enamido)ethyl N-{3-[({[2-ethyl-3-hydroxy-2(hydroxymethyl)propoxy]carbonyl}amino)methyl]-3,5,5-trimethylcyclohexyl}carbamate) contains hydrogen bond active site and light-initiated C=C. We introduced it as a branch chain block into poly(ε-caprolactone) (PCL). By feeding and monitoring the reaction process, we synthesized a large number of polyurethane elastomers, hydrogen bonds PCL-based elastomer (HPE), which contain a large number of dynamic hydrogen bonds. Under UV irradiation, PEMTC can make HPE molecules aggregate and cross-link, improve the degree of internal hydrogen bonding interaction of HPE materials and endow HPE materials with good elasticity, toughness, heat resistance and shape memory ability. After 270 nm UV irradiation, the elongation at break of HPE materials decreased from 607.14-1463.95% to 426.60-610.36%, but the strength at break of HPE materials increased from 3.36-13.52 to 10.28-41.52 MPa, and the toughness increased from 16.36-129.71 to 40.48-172.22 MJ m-3. In addition, the highest shape fixation rate of HPE after UV irradiation was 98.0%, and the recovery rate was 93.7%.
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Project description:Star-shaped cyclophosphazene (ACP) was employed as covalent crosslinker to form a rigid segment in polyurethanes network, to enhance the mechanical performance and to add extra flame retardant property. The effects of different ACP contents on the shape memory ability and fire resistance performance of polyurethane (PU) were studied. Tensile tests suggested high flexibility of the PUs with the maximum elongation-at-break of 161.59%. Dynamic mechanical analysis (DMA) indicated good shape recovery ratio of 72.58% after more than three repeated cycles. Under thermal treatment, the temporary shape could recover to its original state in 10 s. The peak heat release rate (pHRR), total heat released (THR) and temperature at pHRR (Tp) of flame-retardant shape memory polyurethane (FSPU) by micro-combustion calorimeter (MCC) was as low as 183.2 W/g, 21.4 KJ/g, 330.8 °C respectively, suggesting good inherent fire-resistant performance. As amine-containing crosslinkers are one of the most common building units in thermosetting polymers, we anticipate that our finding will have significant benefits beyond shape memory and fire-resistance.
| S-EPMC7240373 | biostudies-literature
Project description:We have previously shown the suitability of aerogels as scaffolds for neuronal cells. Here, we report on the use of superelastic shape memory polyurethane aerogels (SSMPA). SSMPA have a distinctly different stiffness than previously reported aerogels. The soft and deformable nature of SSMPA allowed for radial compression of the aerogel induced by a custom designed apparatus. This radial compression changed the pore diameter and surface roughness (Sa) of SSMPA, while maintaining similar stiffness. Two varieties of SSMPA were used, Mix-14 and Mix-18, with distinctly different pore diameters and Sa. Radial compression led to a decreased pore diameter, which, in turn, decreased the Sa. The use of custom designed apparatus and two types of SSMPA allowed us to examine the influence of stiffness, pore size, and Sa on the extension of processes (neurites) by PC12 neuronal cells. PC12 cells plated on SSMPA with a higher degree of radial compression extended fewer neurites per cell when compared to other groups. However, the average length of the neurites was significantly longer when compared to the unrestricted group and to those extended by cells plated on SSMPA with less radial compression. These results demonstrate that SSMPA with 1.9 µm pore diameter, 1.17 µm Sa, and 203 kPa stiffness provides the optimum combination of physical parameters for nerve regeneration.
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Project description:A green fabrication process (organic solvent-free) of artificial scaffolds is required in tissue engineering field. In this work, a series of aligned three-dimensional (3D) scaffolds are made from biodegradable waterborne polyurethane (PU) emulsion via directional freeze-drying method to ensure no organic byproducts. After optimizing the concentration of polymer in the emulsion and investigating different freezing temperatures, an aligned PUs scaffold (PU14) generated from 14?wt% polymer content and processed at -196°C was selected based on the desired oriented porous structure (pore size of 32.5?±?9.3??m, porosity of 92%) and balanced mechanical properties both in the horizontal direction (strength of 41.3?kPa, modulus of 72.3?kPa) and in the vertical direction (strength of 45.5?kPa, modulus of 139.3?kPa). The response of L929 cells and the regeneration of muscle tissue demonstrated that such pure material-based aligned 3D scaffold can facilitate the development of orientated cells and anisotropic tissue regeneration both in vitro and in vivo. Thus, these pure material-based scaffolds with ordered architecture have great potentials in tissue engineering for biological anisotropic tissue regeneration, such as muscle, nerve, spinal cord and so on.
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Project description:Injectable biomaterials are increasingly being explored to minimize risks and complications associated with surgical implantation. We describe a strategy for delivery via conventional needle-syringe injection of large preformed macroporous scaffolds with well-defined properties. Injectable 3D scaffolds, in the form of elastic sponge-like matrices, were prepared by environmentally friendly cryotropic gelation of a naturally sourced polymer. Cryogels with shape-memory properties may be molded to a variety of shapes and sizes, and may be optionally loaded with therapeutic agents or cells. These scaffolds have the capability to withstand reversible deformations at over 90% strain level, and a rapid volumetric recovery allows the structurally defined scaffolds to be injected through a small-bore needle with nearly complete geometric restoration once delivered. These gels demonstrated long-term release of biomolecules in vivo. Furthermore, cryogels impregnated with bioluminescent reporter cells provided enhanced survival, higher local retention, and extended engraftment of transplanted cells at the injection site compared with a standard injection technique. These injectable scaffolds show great promise for various biomedical applications, including cell therapies.
| S-EPMC3511752 | biostudies-literature
Project description:This article presents data from the investigation of the thermal characteristics and mechanical behaviors of twelve different compositions of a polyurethane shape memory polymer (SMP). Each of the SMP compositions has a unique molar ratio of three monomers: (i) hexamethylene diisocyanate (HDI), (ii) N,N,N',N'-Tetrakis(2-Hydroxypropyl)ethylenediamine (HPED), and (iii) Triethanolamine (TEA). The thermal characteristic datasets for each composition include the glass transition temperatures, as obtained from differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA), and the thermal degradation thresholds, as found from thermogravimetric analysis (TGA). The mechanical behaviors of the SMPs are represented by the failure stresses and strains, as obtained by cyclic tensile testing and failure testing, respectively. The interpretation of these measurements as well as a discussion of the potential usage of candidate SMP compositions for medical devices can be found in the companion article by Kunkel et al. (2018) [1], "Synthesis and characterization of bio-compatible shape memory polymers with potential applications to endovascular embolization of intracranial aneurysms."
| S-EPMC7495509 | biostudies-literature