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A bimetallic Rh<jats:sup>I<\/jats:sup>\u2013Pt<jats:sup>II<\/jats:sup> complex containing an especially designed multidentate phosphine olefin ligand is capable of catalytically detoxifying these nitrogen oxides in the presence of hydrogen to form water and dinitrogen as benign products. The catalytic reactions were performed at room temperature and low pressures (3\u20134\u2005bar for combined nitrogen oxides and hydrogen gases). A turnover number (TON) of 587 for the reduction of nitrous oxide (N<jats:sub>2<\/jats:sub>O) to water and N<jats:sub>2<\/jats:sub> was recorded, making these Rh<jats:sup>I<\/jats:sup>\u2013Pt<jats:sup>II<\/jats:sup> complexes the best homogeneous catalysts for this reaction to date. Lower TONs were achieved in the conversion of nitric oxide (NO, TON=38) or nitrogen dioxide (NO<jats:sub>2<\/jats:sub>, TON of 8). These unprecedented homogeneously catalyzed hydrogenation reactions of NO<jats:sub>x<\/jats:sub> were investigated by a combination of multinuclear NMR techniques and DFT calculations, which provide insight into a possible reaction mechanism. The hydrogenation of NO<jats:sub>2<\/jats:sub> proceeds stepwise, to first give NO and H<jats:sub>2<\/jats:sub>O, followed by the generation of N<jats:sub>2<\/jats:sub>O and H<jats:sub>2<\/jats:sub>O, which is then further converted to N<jats:sub>2<\/jats:sub> and H<jats:sub>2<\/jats:sub>O. The nitrogen\u2212nitrogen bond\u2010forming step takes place in the conversion from NO to N<jats:sub>2<\/jats:sub>O and involves reductive dimerization of NO at a rhodium center to give a hyponitrite (N<jats:sub>2<\/jats:sub>O<jats:sub>2<\/jats:sub><jats:sup>2\u2212<\/jats:sup>) complex, which was detected as an intermediate.<\/jats:p>","DOI":"10.1002\/anie.202109642","type":"journal-article","created":{"date-parts":[[2021,9,12]],"date-time":"2021-09-12T18:04:33Z","timestamp":1631469873000},"page":"25372-25380","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":40,"title":["Reduction of Nitrogen Oxides by Hydrogen with Rhodium(I)\u2013Platinum(II) Olefin Complexes as Catalysts"],"prefix":"10.1002","volume":"60","author":[{"given":"Pascal","family":"Jurt","sequence":"first","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6800-3211","authenticated-orcid":false,"given":"Anne Sofie","family":"Abels","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juan Jos\u00e9","family":"Gamboa\u2010Carballo","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"},{"name":"Higher Institute of Technologies and Applied Sciences (InSTEC) University of Havana  Ave. S. Allende 1110 10600 Havana Cuba"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Israel","family":"Fern\u00e1ndez","sequence":"additional","affiliation":[{"name":"Departamento de Qu\u00edmica Org\u00e1nica I and Centro de Innovaci\u00f3n en Qu\u00edmica Avanzada (ORFEO-CINQA) Facultad de Ciencias Qu\u00edmicas Universidad Complutense de Madrid  28040 Madrid Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gr\u00e9goire","family":"Le Corre","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Marcel","family":"Aebli","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Matthew G.","family":"Baker","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Frederik","family":"Eiler","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fabian","family":"M\u00fcller","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Michael","family":"W\u00f6rle","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ren\u00e9","family":"Verel","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"S\u00e9bastien","family":"Gauthier","sequence":"additional","affiliation":[{"name":"Univ. Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes)\u2014UMR 6226  F-35000 Rennes France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5912-509X","authenticated-orcid":false,"given":"Monica","family":"Trincado","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Thomas L.","family":"Gianetti","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"},{"name":"Department of Chemistry and Biochemistry University of Arizona, Tucson  1306 E. 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