Rational Design of Bioinspired Nucleobase‐Containing Polymers as Tough Bioplastics and Ultra‐Strong Adhesives

The development of polymeric materials from bio-based feedstocks is highly urgent due to growing environmental concerns and the rapid depletion of limited fossil resources. However, bio-based polymeric materials usually possess only moderate performance, drastically undermining their potential applicability. Herein, bioinspired nucleobase-containing polymers with eminent toughness and outstanding adhesive properties by harnessing the complementary hydrogen-bonding (H-bonding) interactions are developed. Efficient thiol-ene polymerization is carried out to produce the nucleobase-functionalized homopolymers and statistical copolymers. In contrast to the individual homopolymers, the supramolecular mixtures of the homopolymers display much better energy dissipation and damping capacity on account of intermolecular complementary H-bonding interactions. More remarkably, the nucleobase-containing copolymers possessing both inter- and intramolecular complementary H-bonding interactions exhibit outstanding toughness as high as 73.8 MJ m−3. In addition to the outstanding mechanical properties, the unique interfacial adhesive propensity of nucleobases endows the polymeric materials with an ultra-strong adhesion strength as high as 16.2 MPa. This work represents an important and universal bioinspired strategy to construct robust polymeric materials by rationally designing both inter- and intramolecular H-bonding networks.