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Browsing by Author "Johnson, Richard Kwesi"

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    TEMPO-oxidized Nanocelluloses: Surface Modification and use as Additives in Cellulosic Nanocomposites
    Johnson, Richard Kwesi (Virginia Tech, 2010-08-18)
    The process of TEMPO-mediated oxidation has gained broad usage towards the preparation of highly charged, carboxyl-functionalized polysaccharides. TEMPO-oxidized nanocelluloses (TONc) of high surface charge and measuring 3 to 5 nm in width have been recently prepared from TEMPO-oxidized pulp. This study examines as-produced and surface-hydrophobized TONc as reinforcing additives in cellulosic polymer matrices. In the first part of the work, covalent (amidation) and non-covalent (ionic complexation) coupling were compared as treatment techniques for the hydrophobization of TONc surfaces with octadecylamine (ODA). Subsequently, TONc and its covalently coupled derivative were evaluated as nanofiber reinforcements in a cellulose acetate butyrate (CAB) matrix. The properties of the resulting nanocomposites were compared with those of similarly prepared ones reinforced with conventional microfibrillated cellulose (MFC). It was found that both ionic complexation and amidation resulted in complete conversion of carboxylate groups on TONc surfaces. As a result of surface modification, the net crystallinity of TONc was lowered by 15 to 25% but its thermal decomposition properties were not significantly altered. With respect to nanocomposite performance, the maximum TONc reinforcement of 5 vol % produced negligible changes to the optical transmittance behavior and a 22-fold increase in tensile storage modulus in the glass transition region of CAB. In contrast, hydrophobized TONc and MFC deteriorated the optical transmittance of CAB by ca 20% and increased its tensile storage modulus in the glass transition region by only 3.5 and 7 times respectively. These differences in nanocomposite properties were attributed to homogeneous dispersion of TONc compared to aggregation of both the hydrophobized derivative and the MFC reference in CAB matrix. A related study comparing TONc with MFC and cellulose nanocrystals (CNC) as reinforcements in hydroxypropylcellulose (HPC), showed TONc reinforcements as producing the most significant changes to HPC properties. The results of dynamic mechanical analysis and creep compliance measurements could be interpreted based on similar arguments as those made for the CAB-based nanocomposites. Overall, this work revealed that the use of TONc (without the need for surface hydrophobization) as additives in cellulosic polymer matrices leads to superior reinforcing capacity and preservation of matrix transparency compared to the use of conventional nanocelluloses.
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    Wetlaid Cellulose Fiber-Thermoplastic Hybrid Composites - Effects of Lyocell and Steam Exploded Wood Fiber Blends
    Johnson, Richard Kwesi (Virginia Tech, 2004-06-18)
    Fiber hybridization involves the blending of high and low performance fibers in a common matrix to yield a composite with a balance of properties that cannot be achieved by using either fiber alone. In this study, the random wetlay process was used as a compounding method to investigate the effects of fiber hybridization on the mechanical, viscoelastic, and sorption characteristics of steam-exploded wood (SEW) and lyocell (high performance regenerated cellulose) fiber-reinforced polypropylene (PP) composites. The two fiber types were blended in varying proportions within a fixed total fiber content of 50 wt. % and compared with non-hybrid lyocell- and SEW-PP controls. Using PP matrix as basis, it was observed that moduli of all composites generally increased with increasing lyocell concentration, ranging from a minimum 66 % for SP 50 (SEW/PP control) to a maximum 233 % for LP 50 (lyocell/PP control). Ultimate strengths on the other hand, declined for SP 50 but increased with the inclusion of lyocell fibers. Comparisons of hybrid (having 5 - 20 wt % lyocell) with non-hybrid (having 25 - 50 wt. % lyocell) composites revealed a surprisingly greater strength and modulus-building efficiency (by as much as 2.6 times) in the hybrid composites. This observation indicated possible synergism between lyocell and SEW. Analyses of composite property gains as a function of fiber cost also showed greater cost benefits (highest for tensile modulus) in favor of hybridization. The advantages of fiber hybridization on composite properties were again evident under dynamic mechanical analysis where no significant differences in the storage moduli were found between a hybrid composite with 20 wt. % lyocell and a non-hybrid composite with 50 wt. % lyocell loading. Application of the time-temperature superposition principle (TTSP) made it possible to predict storage moduli over extended frequencies for PP and its composites. Comparison of shift factor versus temperature plots revealed decreasing relaxation times of PP with increasing lyocell concentration, which indicated that PP interacted better with lyocell than with SEW fibers. Finally, it was observed from sorption tests that hybrid composites absorbed less moisture than non-hybrid counterparts of either fiber type. The reasons for this observation were not apparent. It is however possible that moisture transport mechanisms within the composites may have been modified as a result of hybridization.