Polymer Deconstruction and Redesign Strategies for Plastics Recycling

ABSTRACT Advancing plastics recycling requires both the selective deconstruction of existing polymers and the design of new materials that enable efficient reuse without loss of performance. This perspective highlights an integrated approach that is rooted in polymer chemistry, catalysis, and process engineering which can enable a circular plastics economy. We outline recent advances in catalytic, solvolytic, and enzymatic pathways for plastic deconstruction, and examine the molecular design principles driving next‐generation recyclable‐by‐design and bio‐based polymers. Despite these advances, major knowledge gaps remain in understanding the evolution of polymer morphology and catalyst structure during deconstruction, assessing deconstruction processes with realistic polymers, and offering redesigned polymers with competitive cost and environmental advantage over conventional plastics. United States Department of Energy (U.S. DOE) national laboratories offer unique capabilities to address these challenges through in situ and operando characterization, high‐throughput experimentation, environmental studies, technoeconomic and life cycle assessment, scale‐up support, and collaboration networks. Advances made in understanding plastic deconstruction mechanisms and structure‐property correlations of redesigned polymers inform emerging research directions including autonomous experimentation, real‐time feedback‐enabled process optimization, and protein engineering for enzymatic depolymerization.