Robust Itaconic Acid-Based Polymer Adhesive Nanocomposites Containing Bioinspired Multiple Hydrogen Bonds at the Polymer-Nanofiller Interface

Worldwide efforts have been continuously devoted to transforming biomass into distinct polymer materials due to the constant depletion of limited fossil resources. However, widespread applications of biomass-based materials still warrant further improvement of the mechanical properties, not limited to current strategies, including copolymerization or blending with rigid blocks. Herein, bioinspired multiple hydrogen bonds of complementary nucleobases were successfully incorporated into itaconic acid-based polymer adhesive nanocomposites at the polymer-nanofiller interface. The complementary nucleobases enable the relaxation of interfacial stress efficiently through the dissociation/reassociation of hydrogen bonds at the polymer-nanofiller interface. For the polymer matrix, nucleobase-containing itaconic acid-based polymers prepared via thiol-ene addition polymerization only present moderate adhesive strengths. Adhesive properties were enhanced by introducing core-cross-linked nanoparticles with variable complementary nucleobases in the corona, leading to the adhesive strength as high as 10.6 MPa. The robust adhesive properties of the nanocomposites are mainly due to the high activation energy of the supramolecular network. The strategy developed here underscores the significance of the interfacial interaction for enhancing the properties of adhesive nanocomposites.

Automated summary

This study presents a method to incorporate complementary nucleobases into itaconic acid-based polymer adhesive nanocomposites. The introduction of complementary nucleobases enables efficient relaxation of interfacial stress through the dissociation/reassociation of hydrogen bonds, resulting in improved adhesive properties. Additionally, the adhesive strength can be further enhanced by introducing core-cross-linked nanoparticles with different complementary nucleobases.