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However, metal\u2013metal interactions between dual single atoms and their effects on Cu evolution after exposure to different environmental molecules remain underexplored. Herein, we synthesized bimetallic Cu\u2010Y\/Beta catalysts with dual single\u2010atom Cu and Y sites and monometallic Cu\u2010Beta catalysts with isolated Cu sites in dealuminated Beta zeolites. By varying Cu and Y compositions, diatomic interactions were studied under H\n                    <jats:sub>2<\/jats:sub>\n                    and ethanol atmospheres. With 6 wt% Y loading, approximately 0.4 wt% of Cu species in Cu\u2010Y\/Beta remained partially oxidized as Cu(I) after reduction in pure H\n                    <jats:sub>2<\/jats:sub>\n                    at 350 \u00b0C, in contrast to the full transition to metallic Cu observed in Cu\u2010Beta. Combining X\u2010ray absorption spectroscopy with kinetic studies revealed that metallic Cu became the predominant species after reduction with H\n                    <jats:sub>2<\/jats:sub>\n                    as Cu loading increased from 0.4 to 1.7 wt%, quadrupling the initial ethanol dehydrogenation rate and demonstrating the dominant role of Cu(0) sites. Scanning transmission electron microscopy and density functional theory simulations indicated spatial proximity between dual single\u2010atom Cu and Y sites and elucidated Cu speciation controlled by diatomic interactions.\n                  <\/jats:p>","DOI":"10.1002\/anie.202514920","type":"journal-article","created":{"date-parts":[[2025,9,29]],"date-time":"2025-09-29T11:01:47Z","timestamp":1759143707000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Cu Evolution over Bimetallic Cu\u2010Y\/Beta Zeolite Under H\n                    <sub>2<\/sub>\n                    and Ethanol Atmospheres: Unveiling the Role of Diatomic Metal\u2013Metal Interactions"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5210-9708","authenticated-orcid":false,"given":"Junyan","family":"Zhang","sequence":"first","affiliation":[{"name":"Manufacturing Science Division Oak Ridge National Laboratory  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\u201cRiver\u201d","family":"Samad","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering The University of Alabama  Tuscaloosa AL 35487 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"James W.","family":"Harris","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering The University of Alabama  Tuscaloosa AL 35487 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kinga A.","family":"Unocic","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering NC State University  Raleigh NC 27695 USA"},{"name":"Center for Nanophase Materials Sciences Oak Ridge National Laboratory  Oak Ridge TN 37830 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Evan C.","family":"Wegener","sequence":"additional","affiliation":[{"name":"Chemical Science and Engineering Division Argonne National Laboratory  Lemont IL 60439 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shan","family":"Jiang","sequence":"additional","affiliation":[{"name":"Davidson School of Chemical Engineering Purdue University West Lafayette IN 47907 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenbo","family":"Li","sequence":"additional","affiliation":[{"name":"Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center School of Chemistry and Molecular Engineering East China University of Science and Technology  Shanghai 200237 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jeffrey T.","family":"Miller","sequence":"additional","affiliation":[{"name":"Davidson School of Chemical Engineering Purdue University West Lafayette IN 47907 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Felipe","family":"Polo\u2010Garzon","sequence":"additional","affiliation":[{"name":"Chemical Sciences Division Oak Ridge National 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