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This study aimed to develop cellulose-based polymer matrices as controlled release devices for plant-based insect repellents and attractants, with the aim of finding sustainable and environmentally friendly pest control methods for agricultural applications. Citronellol, terpineol and methyl salicylate were the selected active compounds for this study. Their compatibility with cellulose diacetate was predicted using Hansen Solubility Parameters, which predicted terpineol as the most compatible with cellulose diacetate, followed by methyl salicylate and citronellol. This was consistent with the plasticization efficiency trend from DMA results of solvent cast cellulose diacetate films containing the active compounds. The chemical identity of the films and cellulose diacetate-active compound intermolecular interactions were verified by FTIR. TGA demonstrated the thermal stability of cellulose diacetate/active compound/clay formulations at temperatures not exceeding 170 °C. Cellulose diacetate/organoclay nanocomposite matrices containing the active compounds at 35 wt-% were prepared by twin screw extrusion compounding, with the active compounds also functioning as plasticizers. The amount of active compound in the strands was determined by solvent extraction and TGA. Both methods showed that small amounts of active compound were lost during the compounding process. SEM demonstrated the effect of organoclay on the internal morphology of the matrix, whereas TEM showed clay dispersion and intercalation within the matrix. The matrix served as a reservoir for the active compounds while simultaneously controlling their release into the environment. Release profiles, obtained through oven ageing at 40 °C for 70 days, were fitted to existing Log-logistic and Weibull models, and novel Diffusion and Modified Weibull release models. Citronellol was released the fastest, followed by methyl salicylate and terpineol. The findings suggest that cellulose diacetate/organoclay strands are promising controlled-release matrices for pest control purposes.

This article belongs to the Special Issue Thermal and Rheological Characterization of Polymeric Materials [Abstract] Poly(lactic acid) (PLA) is an attractive candidate for replacing petrochemical polymers because it is fully biodegradable. This study investigated the potential of PLA as a sustainable and environmentally friendly alternative material that can be developed into commercially viable wearable mosquito repellent devices with desirable characteristics. PLA strands containing DEET and IR3535 were prepared by twin screw extrusion compounding and simultaneously functioned as plasticizers for the polymer. The plasticizing effect was investigated by thermal and rheological studies. DSC studies showed that the addition of DEET and IR3535 into PLA strands reduced the glass transition temperature consistent with predictions of the Fox equation, thus proving their efficiency as plasticizers. The rheology of molten samples of neat PLA and PLA/repellents blends, evaluated at 200 °C, was consistent with shear-thinning pseudoplastic behaviour. Raman studies revealed a nonlinear concentration gradient for DEET in the PLA strand, indicating non-Fickian Type II transport controlling the desorption process. Release data obtained at 50 °C showed initial rapid release followed by a slower, near constant rate at longer times. The release rate data were fitted to a novel modification of the Peppas-Sahlin desorption model This work was financially supported from the Deutsche Forschungsgemeinschaft (DFG), Germany [Grant number AN 212/22-2] and University of Pretoria (UP) Postdoctoral Fellowship programme. The research has been also supported by Spanish MINECO grant MTM2017-82724-R through the ERDF Deutsche Forschungsgemeinschaft (DFG); AN 212/22-2 https://www.mdpi.com/journal/molecules/special_issues/Thermal_Rheological_Polymeric_Materials