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Here, we report a spatially confined relay catalysis strategy enabled by Ru single\u2010atom\u2010anchored MOR zeolite (Ru\n                    <jats:sub>1<\/jats:sub>\n                    @MOR), which achieves a maximum C\n                    <jats:sub>4<\/jats:sub>\n                    alkane selectivity of 63.4% and a production rate of 4516.4\u00a0mmol g\n                    <jats:sub>Ru<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    in the hydrocracking of low\u2010density polyethylene, outperforming reported catalysts to date. Combined AC HAADF\u2010STEM, solid\u2011state NMR, and density functional theory calculations demonstrated that isolated Ru\n                    <jats:sub>1<\/jats:sub>\n                    sites are coordinatively situated on the inner surface of MOR, forming Ru\u2500O\u2500Si and Ru\u2500O\u2500Al linkages, which enhance the electrophilicity of framework Al sites and the Br\u00f8nsted acidity strength of adjacent bridging hydroxyl groups, thereby endowing the catalyst with improved hydride abstraction capability while retaining the intrinsic carbenium\u2010ion\u2011mediated cracking pathway. Life\u2011cycle assessment further substantiates the minimal operating cost and environmental impacts of this system, and a techno\u2011economic projection for a 10\u00a0000\u2010tonne\u2010per\u2010year butane facility can yield annual alkane revenues exceeding US$1.5 million. This work provides a retrosynthesis\u2010inspired, atom\u2010economical paradigm for plastic waste valued, highlighting the role of precisely engineered single\u2011atom\/zeolite interfaces in selectivity toward targeted hydrocarbon fractions.\n                  <\/jats:p>","DOI":"10.1002\/anie.1866514","type":"journal-article","created":{"date-parts":[[2026,9,16]],"date-time":"2026-09-16T06:35:39Z","timestamp":1789540539000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ru Single\u2010Atom Anchored Zeolite for Selective Upcycling of Polyolefins Into Butanes"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-7736-8932","authenticated-orcid":false,"given":"Minhao","family":"Tang","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics Center for Carbon Neutral Chemistry Institute of Chemistry 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Interface and Thermodynamics Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Zeng","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rongxiang","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yusi","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory 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