Construction of Biomass Tea Polyphenol-Functionalized Halloysite Nanotubes Enabling Green and Sustained-Release Antioxidants for Highly Antiaging Elastomers

The strategy of using sustainable biomass resources instead of traditional petrochemical products has been established as an environmentally friendly way to achieve the "green rubber" industry. Meanwhile, rubber antioxidants possessing high efficiency, long-lasting protection, migration resistance, and green multifunctional properties have attracted intensive investigation for rubber protection. Herein, a naturally extracted substance of tea polyphenol (TP)-functionalized halloysite nanotubes (HNTs), which generates the slow release of free-radical capturing activity and excellent interfacial interaction in the natural rubber matrix, is fabricated by vacuum-pumping and surface-decorating methods (denoted as HNTs-s-TP). Interestingly, the nontoxic and natural antioxidant HNTs-s-TP exhibited remarkable thermo-oxidative aging resistance and stability in a natural rubber (NR) matrix compared to that of TP directly pumped into the tubes due to the further modification of the chemical anchor TP on the outer surface of HNTs. In addition, we have systematically investigated the mechanism for highly efficient and sustainable antioxidation in the rubber matrix via the natural antioxidant HNTs-s-TP derived from the constructed galloyl structure. We envision that this new natural antioxidant fabrication technology will provide significant insights into the innovation for the construction of green and eco-friendly functionalized rubber additives.