The objective of this thesis was to further develop the polymer composite system consisting of cellulose acetate butyrate (CAB) and high modulus, continuous, regenerated cellulose fiber (lyocell). Of particular concern were both the interfacial adhesion between the fiber and matrix and the consolidation process in the manufacture of these composite materials. Interfacial adhesion was found to be substantial due to the relative lack of the fiber pull-out phenomenon observed after tensile failure in the unmodified fiber composites. This result was then supported in the second study in which similar unmodified fiber composites experienced very little fiber pull out with evidence of a large amount of cohesive failure of the matrix accompanied by matrix particles adhering to the fiber surfaces. Void volume formation was mitigated to a small extent by the use of optimal consolidation conditions. Composites formed at moderate temperature (200 °C), low consolidation pressure (11.8 p.s.i.) and high consolidation time (13 min.) were found to have the lowest void volume formation of ca. 2.8 %. These composites were generally found to have the highest interfacial shear strength, ca. 16 MPa. A tensile modulus of 22 GPa and an ultimate strength of 246 MPa was obtained for this composite having a fiber volume content of ca. 62 %. / Master of Science

Thermoplastic blends of several biodegradable polymers with lignin (L) and lignin esters were prepared by solvent casting and melt processing. Among the biodegradable thermoplastics were cellulose acetate butyrate (CAB), poly-hydroxybutyrate (PHB), poly-hydroxybutyrate-co-valerate (PHBV), and a starch-caprolactone blend (SCL). Lignin esters included acetate (LA), butyrate (LB), hexanoate (LH), and laurate (LL). Blend characteristics were analyzed in terms of thermal and mechanical properties. The results indicate widely different levels of interaction between two polymer constituents. Melt blended samples of CAB/LA and CAB/LB were compatible on a 15-30 nm scale when probed by dynamic mechanical thermal analysis, and the glass transition temperatures of the blends followed Fox equation, whereas those of CAB/LH and CAB/LL showed distinct broad transitions on the same scale. Melt blending produced well dispersed phases whereas large phase separation evolved out of solvent castings. Crystallinity and melting points of PHB and PHBV were affected by the incorporation of lignin component, revealing some interaction between the blend constituents. Blends of SCL with L and LB revealed significant effect on crystallinity and melting temperatures of poly-caprolactone component, revealing polymer-polymer interaction between SCL and lignin components. An increased degree of crystallinity was observed in the case of higher-Tg L compared to lower Tg LB. Improvememt in modulus (and in some cases strength also) was observed in almost all blends types due to the glassy reinforcing behavior of lignin. / Master of Science

Biodegradable thermoplastic composites were prepared using high modulus lyocell fibers and cellulose acetate butyrate (CAB). Two reinforcement fiber types: fabric and continuous fiber tow were used. Fabric had advantages of uniform alignment and easier processing, but lacked the use as a unidirectional reinforcement and a continuous method of matrix application. Three different matrix application methods were screened for both fiber types. Matrix application by suspension of particles in water was not feasible because of particle sizes > 15 &micro m. The other disadvantages were high moisture absorption during matrix application and void formation during consolidation. Melt processing technique using alternating sandwich structure of fabrics and CAB films produced composites with impressive appearance, low void contents and low moisture absorption. However, SEM results revealed interfacial failure and extensive fiber pull out. Relatively larger fiber and matrix regions were present on the scale of 10^-3m. Solution prepregging technique using methyl ethyl ketone (MEK) as a solvent for CAB and continuous fibers as reinforcement produced composites with uniform matrix distribution, high tensile strengths and high modulus, and even wetting of fibers by CAB. A maximum tensile modulus of 21.5 GPa and a maximum strength of 251.7 MPa were achieved for a continuous fiber reinforced composites at a volume fraction of 66.5% compared to 0.8 GPa and 76 MPa for the matrix, respectively. Void contents and water absorption were relatively high compared to comparable carbon fiber composites. / Master of Science