Boosting Polyethylene to Aromatics Upcycling via Microwave Catalysis Over Desilicated HZSM‐5

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Microwave (MW) catalysis offers a unique advantage for plastic upcycling by enabling volumetric energy deposition and preferential heating of MW‐absorbing catalysts. Here, we demonstrate MW‐catalytic upcycling of polyethylene (PE) to aromatics over desilicated HZSM‐5 with controllable pore architecture and acidity. A series of alkali‐treated HZSM‐5‐X (X, alkaline treatment time, hour) was evaluated at 300°C under MW heating. Compared with conventional thermal (TH) heating, MW catalysis markedly enhances aromatics formation during PE upcycling. The optimized HZSM‐5‐3 catalyst achieves an 87 wt.% gas yield with 55 wt.% BTX selectivity. Structural characterization reveals that moderate desilication introduces hierarchical porosity while preserving the MFI framework, whereas excessive desilication reduces crystallinity and weakens micropore confinement. Acidic property analysis indicates a decrease in strong Brønsted acidity accompanied by enriched Lewis acidity after desilication. Time‐on‐stream product evolution confirms accelerated aromatics formation over the optimized catalyst. COMSOL simulations further verify preferential zeolite heating and interfacial hot spots under MW irradiation, providing mechanistic insight into enhanced aromatization performance.