Inorganic-organic hybrid biomaterials have recently attracted much attention because of their widespread use. Silkworm cocoon filaments resulting from sericulture as prospective nanobiomaterials need to be improved, and their properties need to be used for broader purposes. This study was aimed at investigating methods for siliconization of silkworm cocoon filaments and characterizing their cocoon filament properties in terms of their yarn quality, natural dyeing, and antibacterial properties. Three methods of hybridization processes were used in this experiment, namely, in situ natural dyeing of silk yarns while silk filaments were spined, feed engineering through spraying the mulberry leaves with natural dyes and silica-phosphate-M (M = Cu, Fe, or Al) nano pastes, and a combination of both methods. The resulting cocoon filaments were characterized by their siliconization of filament fibers by using FTIR, XRD, and SEM-EDS methods. The yarn tensile strength, color quality, color fastness properties affected by the siliconization of silk filament fibers, and antibacterial properties were also investigated. Results showed that the combination method produced better siliconization of silk fibers, and, consequently, the better siliconization of silk fibers produced better natural dyeing as well as antibacterial properties of their resulting silk yarns.
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