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However, the precise control of intermediate formation and conversion remains challenging due to indiscriminate reactant access to both metal and acid centers. Herein, we utilize the steric hindrance of the sodalite (SOD) framework to exclude bulky benzene and cyclohexene from accessing the metal sites, confining intermediate cyclohexene formation and conversion exclusively to acidic domains and breaking the conventional competitive pathway of cyclohexene migration from metal to adjacent acid sites. Experimentally, Ru nanoparticles were confined within the SOD framework (Ru@SOD), and distal acid sites were introduced by mixing with HY zeolite. In\u2010depth studies reveal that coupled hydrogenation\u2010alkylation reactions over HY domains drive a hydrogen pump effect, which continuously draws active hydrogen spillover from encapsulated Ru sites to sustain efficient benzene hydroalkylation. Such isolated metal\u2010acid architecture redirects the pathway from a competitive hydrogenation\/alkylation to an acid\u2010driven alkylation mediated by hydrogen spillover. At \u223c40% benzene conversion, 75.6% cyclohexylbenzene (CHB) selectivity and a record\u2010high 47.3% CHB yield were achieved with the Ru@SOD + HY catalyst, significantly outperforming reference samples and other catalysts reported to date. This work provides a universal spatial isolation of metal\u2010acid sites to modulate intermediate evolution and optimize selectivity in complex tandem catalysis.<\/jats:p>","DOI":"10.1002\/anie.3006407","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T12:26:29Z","timestamp":1784118389000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Redirecting Reaction Pathway in Tandem Catalysis With Isolated Metal\u2013Acid Architecture"],"prefix":"10.1002","volume":"65","author":[{"given":"Wenfeng","family":"Lang","sequence":"first","affiliation":[{"name":"College of Chemistry State Key Laboratory of Coking Coal Resources Green Exploitation Henan Institute of Advanced Technology Zhengzhou University  Zhengzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kaihang","family":"Sun","sequence":"additional","affiliation":[{"name":"College of 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