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Herein, we report that Fe(OH)<jats:sub><jats:italic>x<\/jats:italic><\/jats:sub> deposition on Pt nanocrystals to give Fe(OH)<jats:sub><jats:italic>x<\/jats:italic><\/jats:sub>\/Pt, enables the selective hydrogenation of nitro groups into amino groups without hydrogenating other functional groups on the aromatic ring. The unique catalytic behavior is identified to be associated with the Fe<jats:sup>III<\/jats:sup>\u2010OH\u2010Pt interfaces. While H<jats:sub>2<\/jats:sub> activation occurs on exposed Pt atoms to ensure the high activity, the high selectivity towards the production of substituted aniline originates from the Fe<jats:sup>III<\/jats:sup>\u2010OH\u2010Pt interfaces. In\u2005situ IR, X\u2010ray photoelectron spectroscopy (XPS), and isotope effect studies reveal that the Fe<jats:sup>3+<\/jats:sup>\/Fe<jats:sup>2+<\/jats:sup> redox couple facilitates the hydrodeoxygenation of the \u2010NO<jats:sub>2<\/jats:sub> group during hydrogenation catalysis. Benefitting from Fe<jats:sup>III<\/jats:sup>\u2010OH\u2010Pt interfaces, the Fe(OH)<jats:sub><jats:italic>x<\/jats:italic><\/jats:sub>\/Pt catalysts exhibit high catalytic performance towards a broad range of substituted nitroarenes.<\/jats:p>","DOI":"10.1002\/anie.202003651","type":"journal-article","created":{"date-parts":[[2020,4,16]],"date-time":"2020-04-16T12:22:13Z","timestamp":1587039733000},"page":"12736-12740","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":144,"title":["Chemoselective Hydrogenation of Nitroaromatics at the Nanoscale Iron(III)\u2013OH\u2013Platinum Interface"],"prefix":"10.1002","volume":"59","author":[{"given":"Yu","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials National &amp; Local Joint Engineering Research Center of Preparation Technology of Nanomaterials College of Chemistry and Chemical Engineering Xiamen University  Xiamen 361005 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruixuan","family":"Qin","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials National &amp; 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