Enhanced Anti‐Migration of Organic Antioxidants via Chitosan‐Encapsulated Ultrathin Intercalated Layered Double Hydroxides Fabricated by a Nucleation‐Encapsulation Coupling Strategy

Abstract Antioxidants play a crucial role in inhibiting polypropylene (PP) oxidative damage and extending polymer lifetime. However, the high migration rate and limited efficiency reduced protection, often requiring overdosing, which raises environmental and health issues. Herein, a more sustainable solution involves an ultrathin antioxidant intercalated layered double hydroxides (LDHs) with chitosan (CS) encapsulation to block the antioxidants migration by tuning CS molecular weight to fully encapsulate LDH unit. The optimized encapsulation inhibits the antioxidants migration without hindering the interlayer diffusion of radicals, thereby providing better protection for PP. The 200kCS‐3L‐LDH/PP with the low molecular weight phenolic antioxidant (3,5‐Di‐tert‐butyl‐4‐hydroxyphenylpropionic acid, abbreviated as DBHP) and encapsulated by CS of MW = 200k at an encapsulation level of 11.6% (actual encapsulation percentage by weight), demonstrates a low migration ratio of 8.17% after 204 h in ethanol at 60 °C and overlong thermal aging resistance time (1920 min) under air, surpassing the conventional and most resistant product currently on the market 1010/PP (46.0% and 640 min, respectively). Such “Russian doll” structure offers a promising way to enhance PP with excellent anti‐migration and antioxidative performance, while providing a valuable strategy for the design and the controlled release if desired of interlayer species in LDHs.