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Ever since the advent of polymer science, polyurethanes have played a huge role in the industrial world. They have been used in endless applications from furniture padding to aircraft coatings, to binders for insensitive munitions. It is therefore important that the chemistry of polyurethanes is well understood as well as the ability to draw relationships between the raw materials selected and the end-use properties of the polymer. Because of the multitude of practical applications, the development of an undergraduate polymer chemistry laboratory focused on polyurethane elastomers is developed and described herein. Polymer chemistry students are exposed to hydroxyterminated polybutadiene (HTPB) polyols as well as di- and multifunctional isocyanates for use in a tin-catalyzed reaction. The effect of catalyst concentration and crosslinking agent on cure time, prepolymer structure on end-use properties, and the effect of crosslink density on physical properties are explored. Students also receive a very important introduction to statistical experimental design. They learn when using statistical experimental design is necessary, and they learn how to manipulate, analyze, and interpret data using two-way ANOVA in Minitab. The development of the lab experiment also led to extrapolating the use of polyurethane elastomers into a new application, the development of a polyurethane spinal muscular atrophy (SMA) brace. SMA is a neurodegenerative disorder that results in the mutation or deletion of the spinal motor neuron gene, resulting in the atrophy of a subject’s spine muscles throughout the continuation of their life. These patients are therefore forced to wear a brace for the entirety of their lives. The current brace technology in use by SMA patients is limited by the fact that SMA affects a very small amount of the population and therefore it is not cost-effective for industry to develop a brace technology designed for these patients. Scoliosis braces such as thoracolumbrosacral orthoses (TLSOs) are too hard and too uncomfortable for patients with SMA; therefore, the polyurethane elastomer was extrapolated to develop a brace with more flexibility and more durability. Two generations of polyurethane elastomeric brace were developed and evaluated by a subject and family with an SMA background. The brace is a much improved technology to the TLSO braces and provides more flexibility, more mobility, greater comfort, and superior modularity to the old technology. An instruction manual is also included with a step-by-step process of how to reproduce the brace.

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Organically modified montmorillonite has been extensively used as nanofiller in studies of polymer layered silicate nanocomposites, promising materials for today's automotive industry because the nano-materials reduce the overall weight of vehicle. However, industrial applications have not followed suit primarily due to cost/performance issues. Supercritical carbon dioxide is promising as an aid in the production of a fully exfoliated polymer layered silicate nanocomposite but has not been fundamentally studied in this regard at present. As the first stage in studies of using supercritical carbon dioxide for aiding the production of thermoplastic elastomer nanocomposites, this thesis investigates the influence of this unique supercritical fluid on the microstructure and surface chemistry of five organically modified clays. Four alkyl-based quaternary ammonium surfactants with different number and length of chains attached and one aromatic quaternary ammonium surfactant were chosen to vary the degree of C02-philicity exhibited by the organoclay. In a high pressure batch vessel, the different organoclays were suspended in the supercritical solvent at temperatures of 50°C and 200°C and pressures of 7.6 MPa and 9.7 MPa for a fixed time and then removed after depressurization at 0.2 MPa/s or 4.8 MPa/s. The structures of these treated clays were characterized by XRD, TEM, DSC, TGA, FT -IR, and SEM, and their chemical properties were analyzed by various methods including atomic absorption spectroscopy, and contact angle measurement. The potential role of water to favor the interaction between scC02 and an organoclay was also investigated. Solute-solvent interactions plasticized the organic modifier while suspended in the supercritical fluid, which resulted in greater chain mobility and further cation exchange. The results indicate that surfactants exhibiting a paraffin-type conformation within the galleries of the clay were most likely to experience significant basal expansion, provided the tilt angle was not already close to being perpendicular to the silicate surface. For those organoclays demonstrating basal expansion, it was noted that the resulting particle size was increased due to enhanced porosity. Water proved useful in clay expansion in certain cases and primarily while operating conditions allowed the co-solvent to remain adsorbed to the clay surface. / Thesis / Master of Applied Science (MASc)

京都大学 / 新制・課程博士 / 博士(薬科学) / 甲第24548号 / 薬科博第165号 / 新制||薬科||18(附属図書館) / 京都大学大学院薬学研究科薬科学専攻 / (主査)教授 山下 富義, 教授 髙倉 喜信, 教授 寺田 智祐 / 学位規則第4条第1項該当 / Doctor of Pharmaceutical Sciences / Kyoto University / DFAM

An efficient interaction formula and a semi-analytical method are developed for calculating the ultimate strength of steel-elastomer sandwich panels under combined in-plane compression and lateral pressure. By using the Galerkin method and extending the semi-analytical method to clamped sandwich panels, the governing equations of sandwich panels have been solved by the Galerkin method. The material nonlinearity is treated by iteration and a three-dimensional mesh. For the load case of pure lateral pressure, the ultimate strength from the semi-analytical method is similar to that from hinge line theory and finite element analysis (FEA). However, the semi-analytical method requires about as much computation as FEA, and it is therefore not suitable for design. Finite element modeling and nonlinear analysis are performed to calculate the ultimate strength of sandwich panels under combined load. The results agree with experimental results. This verifies the accuracy of the current finite element model. The verified finite element model is used to obtain the results for a large set of sandwich panels with various dimensions and load combinations. The FEA results for pure lateral pressure load cases are used to derive a correction factor for the hinge line formula. Statistical analysis confirms that the generalized hinge line formula gives accurate values of ultimate strength of sandwich panels under pure lateral pressure. Except for the pressure-only FEA data points, the other FEA data points are corrected so as not to count the in-plane load carried by the elastomer core. Based on the corrected FEA data points, a general expression is developed for an interaction equation. The resulting equation has a bias of -0.003 and a standard deviation of 0.029. Since the radius of the interaction curve is close to 1, this standard deviation is of the order of 3%, which shows that the ultimate strength given by the equation is very close to the FEA results. The interaction equation is so simple that the ultimate strength of clamped sandwich panels under combined in-plane compression and lateral pressure can be easily calculated. / Ph. D.

Electro-active polymers (EAPs) have emerged as a new class of active materials, which produce large deformations in response to an electric stimulus. EAPs have attractive characteristics of being lightweight, inexpensive, stretchable, and flexible. Additionally, EAPs are conformable, and their properties can be tailored to satisfy a broad range of requirements. These advantages have enabled many target applications in actuation and sensing. A general constitutive formulation for isotropic and anisotropic electro-active materials is developed using continuum mechanics framework and invariant theory. Based on the constitutive law, electromechanical stability of the electro-elastic materials is investigated using convexity and polyconvexity conditions. Implementation of the electro-active material model into a commercial finite element software (ABAQUS 6.9.1, PAWTUCKET, RI, USA) is presented. Several boundary and initial value problems are solved to investigate the actuation and sensing response of isotropic and anisotropic dielectric elastomers (DEs) subject to combined mechanical and electrical loads. The numerical response is compared with experimental results to validate the theoretical model. For the constitutive formulation of the electro-elastic materials, invariants for the coupling between two families of electro-active fibers (or particles) and the applied electric field are introduced. The effect of the orientation of the electro-active fibers and the electric field on the electromechanical coupling is investigated under equibiaxial extension. Advantage of the constitutive formulation derived in this research is that the electromechanical coupling can be illustrated easily by choosing invariants for the deformation gradient tensor, the electro-active fibers, and the electric field. For the electromechanical stability, it is shown that the stability can be controlled by tuning the material properties and the orientation of the electro-active fibers. The electromechanical stability condition is useful to build a stable free energy function and prevent the instabilities (wrinkling and electric breakdown) for the electro-elastic materials. The invariant-based constitutive formulation for the electro-elastic materials including the isotropic and anisotropic DEs is implemented into a user subroutine (UMAT in ABAQUS: user defined material) by using multiplicative decomposition of the deformation gradient and the applicability of the UMAT is shown by simulating a complicated electromechanical coupling problem in ABAQUS/CAE. Additionally, the static and dynamic sensing and actuation response of tubular DE transducers (silicone and polyacrylate materials) with respect to combined electrical and mechanical stimuli is obtained experimentally. It is shown that the silicone samples have better dynamic and static sensing characteristics than the polyacrylate. The theoretical modeling accords well with the experimental results. / Ph. D.