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Plastic waste represents one of the most urgent environmental challenges facing humankind. Upcycling has been proposed to solve the low profitability and high market sensitivity of known recycling methods. Existing upcycling methods operate under energy-intense conditions and use precious-metal catalysts, but produce low-value oligomers, monomers, and common aromatics. Herein, we report a tandem degradation-upcycling strategy to exploit high-value chemicals from polystyrene (PS) waste with high selectivity. We first degrade PS waste to aromatics using ultraviolet (UV) light and then valorize the intermediate to diphenylmethane. Low-cost AlCl 3 catalyzes both the reactions of degradation and upcycling at ambient temperatures under atmospheric pressure. The degraded intermediates can advantageously serve as solvents for processing the solid plastic wastes, forming a self-sustainable circuitry. The low-value-input and high-value-output approach is thus substantially more sustainable and economically viable than conventional thermal processes, which operate at high-temperature, high-pressure conditions and use precious-metal catalysts, but produce low-value oligomers, monomers, and common aromatics. The cascade strategy is resilient to impurities from plastic waste streams and is generalizable to other high-value chemicals (e.g., benzophenone, 1,2-diphenylethane, and 4-phenyl-4-oxo butyric acid). The upcycling to diphenylmethane was tested at 1-kg laboratory scale and attested by industrial-scale techno-economic analysis, demonstrating sustainability and economic viability without government subsidies or tax credits. 

Abstract High‐performance polymers have been concomitant with advanced technology for half a century. With the advancement of synthetic chemistry, the recent development of high‐performance polymers has provided superior properties and enabled wide applications. This article reviews recent research progress in aromatic high‐performance polymers. Particularly, we focus on the synthesis and processing of polyimides, as well as the application in gas separation membranes. We begin with a brief introduction to highlight important history and physiochemical characteristics of polyimides. Then, we review the various synthesis methods, followed by recent advances for improving processability. Finally, we evaluate the use of high‐performance polymers in gas separation membranes with focus given to the key issues of plasticization and aging. Overall, the information presented herein provides an up‐to‐date overview of high‐performance polymers, polyimides particularly, and serves as a guide for further research involving the applications in membrane technologies.