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This study demonstrates the development and characterization of trimetallic Pt\n                    <jats:sub>x<\/jats:sub>\n                    Cr\n                    <jats:sub>x<\/jats:sub>\n                    Ag\n                    <jats:sub>1\u20102x<\/jats:sub>\n                    (\n                    <jats:italic>x<\/jats:italic>\n                    \u2264 0.1) alloys with active Pt\u2013Cr pair\u2010ensembles for non\u2010oxidative ethanol dehydrogenation, leveraging predictions that favorable bonding stabilizes Pt\u2013Cr pairs diluted in Ag. Operando X\u2010ray absorption spectroscopy confirms the preferential formation and stability of Pt\u2013Cr pairings dispersed throughout the Ag matrix, and ambient\u2010pressure X\u2010ray photoelectron spectroscopy shows that Pt\u2013Cr sites have significant activity for ethanol dehydrogenation, while suppressing reaction processes that deactivate binary Pt\u2013Ag and Cr\u2013Ag alloys. 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