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Lewis acids in dichloromethane establish a polar environment that stabilizes carbenium ion intermediates and catalyzes hydride transfer, enabling breaking of polyethylene C\u2212C bonds and forming C\u2212C bonds in alkylation. Here, we show that efficient and selective deconstruction of low\u2010density polyethylene (LDPE) to liquid alkanes is achieved with anhydrous aluminum chloride (AlCl<jats:sub>3<\/jats:sub>) and gallium chloride (GaCl<jats:sub>3<\/jats:sub>). Already at 60\u2009\u00b0C, complete LDPE conversion was achieved, while maintaining the selectivity for gasoline\u2010range liquid alkanes over 70\u2009%. AlCl<jats:sub>3<\/jats:sub> showed an exceptional conversion rate of 5000 \n, surpassing other Lewis acid catalysts by two orders of magnitude. Through kinetic and mechanistic studies, we show that the rates of LDPE conversion do not correlate directly with the intrinsic strength of the Lewis acids or steric constraints that may limit the polymer to access the Lewis acid sites. Instead, the rates for the tandem processes of cracking and alkylation are primarily governed by the rates of initiation of carbenium ions and the subsequent intermolecular hydride transfer. Both jointly control the relative rates of cracking and alkylation, thereby determining the overall conversion and selectivity.<\/jats:p>","DOI":"10.1002\/anie.202319580","type":"journal-article","created":{"date-parts":[[2024,3,4]],"date-time":"2024-03-04T03:05:17Z","timestamp":1709521517000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":25,"title":["Chloride and Hydride Transfer as Keys to Catalytic Upcycling of Polyethylene into Liquid Alkanes"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4506-6583","authenticated-orcid":false,"given":"Wei","family":"Zhang","sequence":"first","affiliation":[{"name":"Institute for Integrated Catalysis Pacific Northwest National Laboratory (PNNL)  Richland Washington 99354 USA"},{"name":"Department of Chemistry and Catalysis Research Center Technical University of Munich (TUM)  Lichtenbergstrasse 4 85747 Garching 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