Synergistic in-situ structural modification and interfacial engineering of lignin toward multifunctional biodegradable films

The use of non-degradable polymer films has raised urgent environmental concerns, prompting the development of biodegradable alternatives with robust mechanical performance; however, the heterogeneous structure and poor interfacial compatibility of lignin often limit its reinforcing efficiency in polymer matrices. Herein, a green γ-valerolactone–gallic acid solvent system was developed for in situ lignin modification during pretreatment, enabling controlled structural reorganization and interfacial engineering within the polyvinyl alcohol (PVA) matrix. GA incorporation increased the density of polar functional groups and enhanced hydrogen bonding interactions with PVA chains, leading to improved interfacial compatibility and a more uniform polymer network. The resulting film demonstrated improved mechanical properties—tensile strength (∼46 MPa), Young’s modulus (0.22 GPa), and toughness (70 MJ·m −3 ). Lignin integration enhanced water resistance and imparted efficient photothermal conversion, enabling stable cyclic heating under solar irradiation. This strategy provides a viable approach for developing biodegradable films that combine mechanical integrity with multifunctionality.