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Here we report the synthesis of self\u2010pillared pentasil (SPP) zeolite microspheres as self\u2010supported catalyst bodies built from nanosheets in a characteristic house\u2010of\u2010cards arrangement. Time\u2010resolved studies reveal that, in a dual\u2010template system containing tetrabutylphosphonium hydroxide (TBPOH) and ethylenediamine (EDA) as co\u2010structure\u2010directing agents, SPP zeolite nanosheets spontaneously assemble into microscale spheres during crystallization while developing their hierarchical architecture. This strategy is not limited to the pure\u2010silica composition but also enables the synthesis of aluminosilicate SPP microspheres with enriched Br\u00f8nsted and Lewis acidity. Diffusion measurements, together with peak\u2010force quantitative nanomechanical mapping (PF\u2010QNM) and nanoindentation analyses, show that the SPP microspheres combine efficient molecular transport with appreciable mechanical robustness. As a proof of concept, we further demonstrate that the aluminosilicate SPP microspheres function as self\u2010supported and recyclable catalysts for polyethylene upcycling, which achieve high conversion, selective formation of liquid hydrocarbons, and excellent structural stability upon reuse. These findings provide a synthetic blueprint for self\u2010supporting structured zeolitic catalysts and highlight their broader potential in catalytic transformations involving bulky molecules.<\/jats:p>","DOI":"10.1002\/anie.1633031","type":"journal-article","created":{"date-parts":[[2026,9,15]],"date-time":"2026-09-15T11:16:27Z","timestamp":1789470987000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Self\u2010Pillared Pentasil Zeolite Microspheres as Self\u2010Supported Catalysts With Enhanced Molecular Diffusion for Waste Plastic Upcycling"],"prefix":"10.1002","author":[{"given":"Siting","family":"Yu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Engineering and Low\u2010Carbon Technology Department of Chemical Engineering Tsinghua University  Beijing 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