Abstract
Bionanocomposites of chitosan and chitosan/carboxymethyl cellulose (CMC) polyelectrolyte complexed materials with graphene oxide (GO) or reduced graphene oxide (rGO) were prepared by thermomechanical processing with excellent levels of dispersion. While GO has a greater affinity with the chitosan polycation, rGO had a more pronounced effect on properties resulting in increased tensile strength, Shore D hardness, and thermal stability of both matrices. Although GO is more hydrophilic than rGO, the former increased more effectively the surface hydrophobicity of the biocomposites regardless of matrix type. GO and rGO changed the α-transition of the biocomposites in a similar manner. The electrochemical properties of the biocomposites were influenced by both nanofiller type and matrix. This research revealed that inclusion of 2D carbon nanomaterials can alter biopolymer interactions and that the phase structure of the biopolymer blend may play a more important role than nanofiller–matrix interactions in determining the overall properties of these bionanocomposites.
Highlights
Compared to traditional synthetic polymers, natural biopolymers such as cellulose, chitin, starch and protein have many advantages such as renewability, wide availability, biodegradability, nontoxicity, and biocompatibility
We have compared the effects of graphene oxide (GO) and reduced graphene oxide (rGO), the latter more hydrophilic than the former, on the properties of polyelectrolyte complexed biopolymer materials
While it is widely believed that nanofiller–matrix interactions are crucial for property enhancement in nanocomposites, our results unexpectedly show that inclusion of GO, which has a greater affinity with chitosan than rGO, did not always yield the most desirable composite properties
Summary
Compared to traditional synthetic polymers, natural biopolymers such as cellulose, chitin, starch and protein have many advantages such as renewability, wide availability, biodegradability, nontoxicity, and biocompatibility. Different chitosan and chitosan/CMC polyelectrolyte complexed materials containing either GO or rGO were prepared by thermomechanical processing This “dry” method has been shown to be cost-effective for processing biopolymers [33,34,35,36] but has scarcely been reported for the preparation of composites of biopolymers and graphene. The strong shear effect during the thermomechanical processing of high-viscosity materials is expected to facilitate the disruption of the original hydrogen-bonding network, the dispersion of the nanomaterials in the matrices, and the interactions between biopolymer chains and between different components. This makes thermomechanical processing more advantageous than widely used solution methods for preparing biopolymer nanocomposites. We discuss multiple factors in such nanocomposite systems that are key in determining the composite material structure and properties providing insights into the design of novel bionanocomposites
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