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Inorganic hydrate-salt filler coated with elastomer containing acidic groups imparts flame and smoke retardancy to thermoplastics while preventing degradation of impact resistance that results from high filler loadings in thermoplastic.
A polymer system has been prepared which has the excellent thermoplastic properties generally associated with polysulfones, and the solvent resistance and thermal stability of aromatic polyimides. This material, with improved processability over the base polyimide, can be processed in the 260-325 C range in such a manner as to yield high quality, tough unfilled moldings; strong, high-temperature-resistant adhesive bonds; and well consolidated, graphite-fiber-reinforced moldings (composities). The unfilled moldings have physical properties that are similar to aromatic polysulfones which demonstrates the potential as an engineering thermoplastic. The adhesive bonds exhibit excellent retention of initial strength levels even after thermal aging for 5000 hours at 232 C. The graphite-fiber-reinforced moldings have mechanical properties which makes this polymer attractive for the fabrication of structural composites.
A modification was formulated to Besseling's Subvolume Method to allow it to use multilinear stress-strain curves which are temperature dependent to perform cyclic thermoplasticity analyses. This method automotically reproduces certain aspects of real material behavior important in the analysis of Aircraft Gas Turbine Engine (AGTE) components. These include the Bauschinger effect, cross-hardening, and memory. This constitutive equation was implemented in a finite element computer program called CYANIDE. Subsequently, classical time dependent plasticity (creep) was added to the program. Since its inception, this program was assessed against laboratory and component testing and engine experience. The ability of this program to simulate AGTE material response characteristics was verified by this experience and its utility in providing data for life analyses was demonstrated. In this area of life analysis, the multiaxial thermoplasticity capabilities of the method have proved a match for the actual AGTE life experience.
The mixed mode interlaminar fracture toughness, G(c), is obtained for the two thermoplastic matrices UDEL P1700 polysulfone and ULTEM polyetherimide by means of edge delamination tensile (EDT) tests on unnotched, eleven-ply graphite fiber reinforced composite specimens. A novel method is used to obtain the stiffness parameter employed in the closed form equation for the calculation of G(c), decreasing the number of stiffness measurements required and simplifying the calculations. The G(Ic) values from double cantilever beam (DCB) measurements on composites of the two thermoplastics were similar to each other, but slightly higher than the G(c) data obtained by EDT. Interfacial resin/fiber failures predominated in both the EDT and DCB tests.
Efforts were directed to develop processing methods to make carbon fiber/thermoplastic fiber preforms that are easy to handle and drapeable, and to consolidate them into low void content laminates. The objectives were attained with the development of the hybrid yarn concept; whereby, thermoplastic fiber can be intimately intermixed with carbon fiber into a hybrid yarn. This was demonstrated with the intermixing of Celion 3000 with a Celanese liquid crystal polymer fiber, polybutylene terepthalate fiber, or polyetheretherketone fiber. The intermixing of the thermoplastic matrix fiber and the reinforcing carbon fiber gives a preform that can be easily fabricated into laminates with low void content. Mechanical properties of the laminates were not optimized; however, initial results indicated properties typical of a thermoplastic/carbon fiber composites prepared by more conventional methods.
The following approaches improved the solvent resistance and raised the Tg of thermoplastics: end-capping aligomers with ethynyl groups; incorporating ethynyl groups pendent along the polymer chain; and correcting polymers containing pendent ethynyl groups with a low molecular weight diethynyl compound. The following conclusions were reached: (1) film and composite properties off an ethynyl-terminated sulfone were better than those of UDEL (trademark); (2) fracture energy of an ethynyl-terminated sulfone was lower than that of UDEL (trademark); (3) residual palladium in the cured ethynyl-terminated sulfone lower the thermooxidative stability of the cured resin; (4) the properties of a phenoxy resin were altered considerably by placing pendent ethynyl groups along the polymer chain; and (5) property trade-offs must be considered when thermoplastics are modified via reactant groups.
The detailed characterization of an experimental thermoplastic polyimidesulfone adhesive based on 3,3 prime-diaminodiphenylsulfone and 3,3 prime,4,4 prime-benzophenone tetracarboxylic dianhydride was studied. Model compounds were also examined. Thermal cyclization of the amide-acid to the imide was studied by a variety of techniques including DSC, TGA, MS, in situ diffuse reflectance-FTIR, and flow mearsurement. Characterizations were continued during the processing of adhesive tapes and the fabrication, bonding, and testing of lap shear specimens. Results provide fundamental insights into the role of cure chemistry, and the effects of residual solvent and volatile produces on processing and performance. These insights and the resulting chemical models should lead to more efficient processing cycles for these and other related thermoplastic adhesive systems.
A polymer system has been prepared which has the excellent thermoplastic properties generally associated with polysulfones, and the solvent resistance and thermal stability of aromatic polyimides. This material, with improved processability over the base polyimide, can be processed in the 260-325 C range in such a manner as to yield high quality, tough unfilled moldings; strong, high-temperature-resistant adhesive bonds; and well consolidated, graphite-fiber-reinforced moldings (composites). The unfilled moldings have physical properties that are similar to aromatic polysulfones which demonstrates the potential as an engineering thermoplastic. The adhesive bonds exhibit excellent retention of initial strength levels even after thermal aging for 5000 hours at 232 C. The graphite-fiber-reinforced moldings have mechanical properties which makes this polymer attractive for the fabrication of structural composites.
Two different types of thermoplastic glassy polymers have been investigated for the effects of thermal annealing on their free volumes. It has been observed that free volumes in glassy polymers decrease asymptotically to a steady level after about four thermal anneals lasting for 24 hours at a temperature about 50 C below their glass transition temperatures. These results indicate that composites incorporating properly annealed thermoplastic matrices may not experience any additional internal stresses due to subsequent thermal excursions experienced while in service.
The detailed characterization of an experimental thermoplastic polyimidesulfane adhesive based on 3,3 prime-diaminodiphenylsulfone and 3,3 prime,4,4 prime-benzophenone tetracarboxylic dianhydride was studied. Model compounds were also examined. Thermal cyclization of the amide-acid to the imide was studied by a variety of techniques including DSC, TGA, MS, in situ diffuse reflectance-FTIR, and flow measurement. Characterizations were continued during the processing of adhesive tapes and the fabrication, bonding, and testing of lap shear specimens. Results provide fundamental insights into the role of cure chemistry, and the effects of residual solvent and volatile produces on processing and performance. These insights and the resulting chemical models should lead to more efficient processing cycles for these and other related thermoplastic adhesive systems.
Method developed for analysis of nonisothermal cold crystallization in thermoplastics. Does not require prior knowledge of isothermal kinetic parameters. Based upon observation: During nonisothermal crystallization at constant rate, relative crystallinity develops with time dependence sigmoidal at low degrees of conversion. Application for method is study of cold crystallization in advanced thermoplastics.
The crystallization kinetics of the thermoplastic resins poly(phenylene sulfide) (PPS) and poly(aryl-ether-ether-ketone) (PEEK) in the presence and in the abscence of carbon fibers was studied. How carbon fiber surfaces in composites affect the crystallization of tough thermoplastic polymers that may serve as matrix resins were determined. The crystallization kinetics of such substances can provide useful information about the crystallization mechanisms and, thus, indicate if the presence of carbon fibers cause any changes in such mechanisms.
A review was made of the principal thermoplastics used to fabricate high performance composites. Neat resin tensile and fracture toughness properties, glass transition temperatures (Tg), crystalline melt temperatures (Tm) and approximate processing conditions are presented. Mechanical properties of carbon fiber composites made from many of these thermoplastics are given, including flexural, longitudinal tensile, transverse tensile and in-plane shear properties as well as short beam shear and compressive strengths and interlaminar fracture toughness. Attractive features and problems involved in the use of thermo-plastics as matrices for high performance composites are discussed.
The single fiber adhesion shear test has been adapted to testing the adhesion between carbon fiber and thermoplastic polymers. Tests of three thermoplastics, polycarbonate, polyphenylene oxide and polyetherimide indicate the shear adhesion strength is significantly less than of an epoxy polymer to the same carbon fiber.
Method developed for preparing readily-processable thermoplastic polyimides by blending linear, high-molecular-weight, polyimic acid solutions in ether solvents with ultrafine, semicrystalline, thermoplastic polyimide powders. Slurries formed used to make prepregs. Consolidation of prepregs into finsihed composites characterized by excellent melt flow during processing. Applied to film, fiber, fabric, metal, polymer, or composite surfaces. Used to make various stable slurries from which prepregs prepared.
A review was made of the principal thermoplastics used to fabricate high performance composites. Neat resin tensile and fracture toughness properties, glass transition temperatures (Tg), crystalline melt temperatures (Tm) and approximate processing conditions are presented. Mechanical properties of carbon fiber composites made from many of these thermoplastics are given, including flexural, longitudinal tensile, transverse tensile and in-plane shear properties as well as short beam shear and compressive strengths and interlaminar fracture toughness.
A continuous powder coating system was developed for coating carbon fiber with LaRC-TPI (Langley Research Center-Thermoplastic Polyimide), a high-temperature thermoplastic polymide invented by NASA-Langley. The coating line developed used a pneumatic fiber spreader to separate the individual fibers. The polymer was applied within a recirculating powder coating chamber then melted using a combination of direct electrical resistance and convective heating to make it adhere to the fiber tow. The tension and speed of the line were controlled with a dancer arm and an electrically driven fiber wind-up and wind-off. The effects of heating during the coating process on the flexibility of the prepreg produced were investigated. The uniformity with which the fiber tow could be coated with polymer also was examined. Composite specimens were fabricated from the prepreg and tested to determine optimum process conditions. The study showed that a very uniform and flexible prepeg with up to 50 percent by volume polymer could be produced with this powder coating system. The coating line minimized powder loss and produced prepeg in lengths of up to 300 m. The fiber spreading was found to have a major effect on the coating uniformity and flexibility. Though test results showed low composite tensile strengths, analysis of fracture surfaces under scanning electron microscope indicated that fiber/matrix adhesion was adequate.
The use of a rubber modified thermoplastic resin has been investigated as a method to improve the impact damage and the Mode I interlaminar fracture toughness of a unidirectional continuous carbon fiber composite. Test results show that the improvement in the fracture toughness is less than expected due to rubber particle agglomeration, poor fiber/matrix adhesion and the induced crystallization of the matrix. These restrictions must be eliminated in order to evaluate the maximum potential of a rubber toughened thermoplastic matrix on a composite's fracture toughness.