Phototunable Lignin Plastics to Enable Recyclability

Abstract The accumulation of non‐degradable petrochemical plastics imposes a significant threat to the environment and ecosystems. We addressed this challenge by designing a new type of phototunable plastics based on the unique lignin chemistry to enable readily end‐life recycling. The advanced material design leveraged the efficient photocatalytic lignin depolymerization by ZnO nanoparticles to build lignin‐polymethyl methacrylate (PMMA)‐ZnO blends. We first demonstrated the highly effective phototunable lignin depolymerization in the complex polymer blend matrix and explored the molecular mechanisms. The technical barriers of mechanical property and recycling processing were then addressed by a new blend design with lignin core grafted with PMMA polymer. The new process has resulted in a new type of PMMA‐ g ‐lignin blend, which significantly improved the mechanical properties, making it comparable to PMMA alone. More importantly, the mechanical properties of the UV‐treated blend decreased drastically in the new design, whereas the properties did not reduce in the non‐grafted blends upon UV exposure. The results highlighted that the new blend design based on graftization maximized the impact of lignin depolymerization on blend structure and recyclability. Based on the results, we developed a process integrating UV and alkaline treatments to recycle PMMA for plastics and fractionated lignin for bioconversion or other applications in the new phototunable plastics.