*Article* **Effective Aging Inhibition of the Thermoplastic Corn Starch Films through the Use of Green Hybrid Filler**

**Di Sheng Lai 1,2, Azlin Fazlina Osman 1,2,\* , Sinar Arzuria Adnan 1,2 , Ismail Ibrahim 1,2 , Midhat Nabil Ahmad Salimi 1,2 and Awad A. Alrashdi <sup>3</sup>**


**Abstract:** Recently, hybrid fillers have been widely used to improve the properties of biopolymers. The synergistic effects of the hybrid fillers can have a positive impact on biopolymers, including thermoplastic corn starch film (TPCS). In this communication, we highlight the effectiveness of hybrid fillers in inhibiting the aging process of TPCS. The TPCS, thermoplastic corn starch composite films (TPCS-C), and hybrid thermoplastic corn starch composite film (TPCS-HC) were stored for 3 months to study the effect of hybrid filler on the starch retrogradation. TPCS-C and TPCS-HC were prepared by casting method with 5 wt% of fillers: nanocellulose (NC) and bentonite (BT). The alteration of the mechanical properties, aging behavior, and crystalline structure of the films were analyzed through the tensile test, Fourier transform infrared (FTIR), X-ray diffraction (XRD), differential scanning calorimetry (DSC), and water absorption analysis. The obtained data were correlated to each other to analyze the retrogradation of the TPCS, which is the main factor that contributes to the aging process of the biopolymer. Results signify that incorporating the hybrid filler (NC + BT) in the TPCS/4BT1NC films has effectively prevented retrogradation of the starch molecules after being stored for 3 months. On the contrary, the virgin TPCS film showed the highest degree of retrogradation resulting in a significant decrement in the film's flexibility. These findings proved the capability of the green hybrid filler in inhibiting the aging of the TPCS.

**Keywords:** thermoplastic starch; nanocellulose; bentonite; biocomposite; aging; retrogradation
