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Mechanics of Biological Polymer Composites
Lomakin, Joseph
Lomakin, Joseph
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Abstract
Cartilage and cuticle are two natural materials capable of remarkable mechanical performance, especially considering the limitations on composition and processing conditions under which they are constructed. Their impressive properties are postulated to be a consequence of their complex multi-scale organization which has commonly been characterized by biochemical and microscopic methods. The objective of this dissertation is to overcome the limitations of such methods with mechanical analysis techniques generally reserved for the study of synthetic polymers. Methods for transient and dynamic mechanical analysis (DMA) of porcine TMJ disc sections and Tribolium castaneum and Tenebrio molitor elytral (modified forewing) cuticle were developed to characterize the mechanical performance of these biomaterials. The TMJ disc dynamic elastic modulus (E') was determined to be a strong function of disc orientation and pretension ranging from 700±240 kPa at (1g pretension) in the mediolateral direction to 73±8.5 MPa (150g preload) in the anteroposterior direction. Analogous mechanical testing was used to understand the relationship between composition and mechanical properties of beetle elytral cuticle at variable stages of maturation (tanning). Untanned elytra of both beetle species were ductile with a Young's modulus (E) of 44±8 MPa, but became brittle with an E of 2400±1100 MPa when fully tanned. Significantly, the E' of the TMJ disc and elytral cuticle exhibited a weak power law increase as a function of oscillation frequency. The exponent of the power law fit (n) was determined to be a sensitive measure of molecular structure within these biomaterials. With increasing cuticular tanning, more so than with drying, the frequency dependence of cuticle E' diminished, suggesting cuticular cross-linking was an important component of tanning, as postulated by the quinone tanning hypothesis. The natural Black phenotype as well as TcADC iRNA suppressed Tribolium cuticle displayed a darker coloration and significantly increased n of 0.047± 0.004, suggesting both cuticles to be less cross-linked, a finding consistent with reduced b-alanine metabolism. Suppression of the tanning enzyme laccase2 (TcLac2) resulted in a pale cuticle with an n of 0.043±0.005, implicating laccases in the formation of both pigments and cross-links during sclerotization. Cuticular cross-linking was increased and n decreased with decreased expression of structural proteins, CP10 and CP20. This work establishes n as an important novel parameter for confirming metabolic pathways within load bearing tissues and for understanding structure function relationships within biological polymer composites. Additionally, Tribolium castaneum elytral indentation modulus (800±200 MPa) was determined by nanoindentation and a 4nm regular hexagonal pattern on the dorsal side of elytra investigated via scanning, transmission and atomic microscopy. Based on studied biological materials, the combination of rigid macromolecules immersed in a ductile matrix was found to be significant in achieving exceptional mechanical performance. Inspired by this biological design principle, the synthesis, properties and structure of Poly(ethylene glycol) diacrylate/agarose semi-interpenetrating network hydrogels were explored. The resulting novel composite materials were 9x stiffer than agarose and 5x tougher than PEGDA alone and showed good biocompatibility, suggesting promise as a scaffold material for tissue engineering constructs for cartilage regeneration.
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2009-01-01
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University of Kansas
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Keywords
Engineering, Materials Science, Engineering, Biomedical, Engineering, Mechanical, dynamic mechanical analysis, frequency sweep, insect cuticle, tribolium