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Herein, we engineered a ZnO\u2010decorated Cu\u2010rich Cu\u2013Zn alloy using a mixed Cu\/Zn oxalate\u2010based supramolecular metal\u2013organic framework precursor with compositionally homogeneous Cu\/Zn mixing. The resulting Cu\u2013Zn catalyst (Cu\u2013Zn|C\u2010oxo|R) maintained &gt;99% CO selectivity and, at 550\u00b0C, delivered a Cu\u2010normalized CO space\u2013time yield (STY) of 1580\u00a0mmol\n                    <jats:sub>CO<\/jats:sub>\n                    \u00a0g\n                    <jats:sub>Cu<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , higher than those of the Cu\u2010only and commercial Cu\u2013Zn\u2013Al benchmarks. Under a high space velocity test, the Cu\u2013Zn|C\u2010oxo|R catalyst remained stable for &gt;50\u00a0h at 550\u00b0C. Operando Cu K\u2010edge x\u2010ray absorption spectroscopy shows that Cu is reduced to a predominantly metallic local environment that persists under RWGS conditions. Complementary in situ x\u2010ray diffraction and electron microscopy identify Cu\u2010rich Cu\u2013Zn alloy domains in contact with ZnO, while in situ diffuse reflectance infrared Fourier transform spectroscopy is consistent with an associative formate\u2010mediated RWGS pathway at these interfaces. Density functional theory calculations further revealed that these interfacial sites favor the formate reaction pathway, providing a molecular\u2010level rationale for the enhanced catalytic activity.\n                  <\/jats:p>","DOI":"10.1002\/anie.4933664","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T03:35:22Z","timestamp":1790825722000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Induced Restructuring of a Supramolecular Metal\u2012Organic Framework Into a Cu\u2500Zn Alloy Catalyst for Reverse Water\u2013Gas Shift"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1182-8332","authenticated-orcid":false,"given":"Vijay K.","family":"Velisoju","sequence":"first","affiliation":[{"name":"Multiscale Reaction Engineering King Abdullah University of Science and Technology (KAUST)  Thuwal Saudi 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