Development of Natural Insect-Repellent Loaded Halloysite Nanotubes and their Application to Food Packaging to Prevent Plodia interpunctella Infestation

The aims of this study were to develop insect-proof halloysite nanotubes (HNTs) and apply the HNTs to a low-density polyethylene (LDPE) film that will prevent Plodia interpunctella (Hubner) (Lepidoptera: Pyralidae), commonly known as Indian mealmoth, from infesting the food. Clove bud oil (CO), an insect repellent, was encapsulated into HNTs with polyethylenimine (PEI) to bring about controlled release of CO. Chemical composition and insecticidal effect of CO were examined. The Fourier transform infrared (FTIR) spectrum of encapsulated CO was confirmed. The surface charges of uncoated HNTs (HNTs/CO) and coated HNTs with PEI by the layer-by-layer (LBL) method (HNTs/CO/LBL) were determined to be -37.23 and 36.33 mV, respectively. HNTs/CO/LBL showed slow, controlled release of CO compared to HNTs/CO. After 30 d, the residual amounts of CO in HNTs/CO and HNTs/CO/LBL were estimated to be 13.43 and 28.66 mg/g, respectively. HNTs/CO/LBL showed the most sustainable repellent effect. HNTs applied to gravure printing ink solution did not affect mechanical, optical, or thermal properties of the developed film. Gravure-printed LDPE film containing HNTs/CO/LBL displayed the greatest preventive effect on insect penetration, indicating its potential for use as insect-resistant food packaging materials.