Extraction of chitin nanofibers and utilization for sustainable composites and foams

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Wu, Jie
Meredith, J. Carson
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Developing renewable materials to reduce the dependence on fossil fuel as a feedstock for a wide range of applications is becoming increasingly acknowledged as important in society. Chitin, the second most abundant biopolymer in nature, is an ideal candidate for diverse applications because of its remarkable properties, such as abundance, renewability, biodegradability, biocompatibility, antibacterial activity, chemical functionality, and high stiffness and strength. Despite these inherent advantages, chitin is currently still underutilized mainly due to its strong molecular interactions, which make it insoluble in common solvents. Currently, its major applications are limited to biomedical engineering, such as tissue engineering, wound dressing and sutures. This thesis aims to explore and enable the potential utilization of chitin in other fields where it may serve as a renewable functional advanced material. Here, a number of novel chitin-based materials were developed successfully without employing chitin dissolution. These include chitin nanofibers (CNFs), porous chitin with tunable structures, chitin-reinforced polymer composites and chitin-stabilized aqueous foams. Moreover, the properties of these materials including interfacial, optical, thermal, and mechanical characteristics were determined, and their potential utilizations were demonstrated. Briefly, in chapter 2, CNFs with diameters of ~20 nm were successfully extracted from crab α-chitin by a high pressure homogenization process. The produced CNFs were dispersed well in water without forming strong network structures due to their electrostatic repulsions. The obtained CNF film has a high residue amount (40%) when heated up to 1000 ˚C. Meanwhile, it exhibited high optical transparency as well as great gas barrier properties. In chapter 3, on the basis of the obtained CNFs in chapter 2, versatile porous structures including oriented sheets and three-dimensional aperiodic nanofiber networks were achieved by using a freeze drying technique. Since the formation of nanofibrous structures cannot be predicted by the widely-used particle encapsulation model, a modified structure formation mechanism was proposed. In chapter 4, the structure-property relationships of the CNF/poly(ethylene oxide)(PEO) nanocomposites were established. We demonstrated that the CNFs formed network structures in PEO matrix and had hydrogen bonding interaction with PEO. The CNFs can greatly enhance the mechanical properties of PEO, such as elastic modulus and tensile strength. In chapter 5, the aqueous foams stabilized by high-aspect-ratio CNFs were developed. The created foams exhibited strong hindrance on film drainage, coalescence and disproportionation. The fibrillated CNFs alone were not able to stabilize air bubbles, but the addition of small amounts of valeric acids in CNF dispersion can make chitin foamable. The results clearly showed that valeric acid modified CNFs reduced the surface tension of aqueous dispersion and were attached at the air-water interface. Overall, this research has provided many new insights for the fabrication, characterization, and utilization of chitin, and has built a solid foundation for further exploiting chitin for diverse applications.
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