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In this study, we design a dual Cu\u2212Cs catalytic system that enables a one\u2010step direct conversion of methanol and methyl acetate\/ethanol into high value\u2010added esters\/aldehydes, with customized chain length and saturation by leveraging the proximity and distribution of Cu\u2212Cs sites. Cu\u2212Cs at a millimeter\u2010scale intimacy triggers methanol dehydrogenation and condensation, involving proton transfer, aldol formation, and aldol condensation, to obtain unsaturated esters and aldehydes with selectivities of 76.3\u2009% and 31.1\u2009%, respectively. Cu\u2212Cs at a micrometer\u2010scale intimacy significantly promotes mass transfer of intermediates across catalyst interfaces and their subsequent hydrogenation to saturated esters and aldehydes with selectivities of 67.6\u2009% and 93.1\u2009%, respectively. Conversely, Cu\u2212Cs at a nanometer\u2010scale intimacy alters reaction pathway with a similar energy barrier for the rate\u2010determining step, but blocks the acidic\u2010basic sites and diverts the reaction to byproducts. More importantly, an unprecedented quadruple tandem catalytic production of methyl methacrylate (MMA) is achieved by further tailoring Cu and Cs distribution across the reaction bed in the configuration of Cu\u2212Cs||Cs, outperforming the existing industrial processes and saving at least 15\u2009% of production costs.<\/jats:p>","DOI":"10.1002\/anie.202314288","type":"journal-article","created":{"date-parts":[[2023,11,21]],"date-time":"2023-11-21T22:28:04Z","timestamp":1700605684000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Leveraging the Proximity and Distribution of Cu\u2212Cs Sites for Direct Conversion of Methanol to Esters\/Aldehydes"],"prefix":"10.1002","volume":"63","author":[{"given":"Wenyao","family":"Chen","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Engineering School of Chemical Engineering East China University of Science and Technology  Shanghai 200237 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