Degradable Poly(vinyl alcohol)‐Based Supramolecular Plastics with High Mechanical Strength in a Watery Environment

Abstract It is challenging to fabricate degradable poly(vinyl alcohol) (PVA)‐based plastics that can be used in watery environments because PVA is soluble in water. In this study, PVA‐based supramolecular plastics with excellent degradability in soil and high mechanical strength in watery environments are fabricated by the complexation of vanillin‐grafted PVA (VPVA), hydrophobic humic acid (HA), and Fe 3+ ions (hereafter denoted as VPVA–HA–Fe complexes). Large‐area PVA‐based plastics can be easily prepared from a solution of VPVA–HA–Fe complexes using a blade‐coating method. The high‐density of hydrogen bonds and coordination interactions, as well as the reinforcement of self‐assembled Fe 3+ ‐chelated HA nanoparticles, facilitate the fabrication of PVA‐based plastics with a breaking strength of ≈85.0 MPa. After immersion in water at room temperature for 7 d, the PVA‐based plastics exhibit a breaking strength of ≈26.2 MPa, which is similar to that of polyethylene in its dry state. Furthermore, owing to the reversibility of the hydrogen bonds and coordination interactions, the VPVA–HA–Fe plastics are recyclable and can be conveniently processed into plastic products with desired shapes. After being placed under soil for ≈108 d, the PVA‐based plastics are completely degraded into nontoxic species without requiring manual interference.