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The ligand\u2013metal bifunctional rhenium catalysts [Re(H)(NO)(PR<jats:sub>3<\/jats:sub>)(C<jats:sub>5<\/jats:sub>H<jats:sub>4<\/jats:sub>OH)] (R=<jats:italic>i<\/jats:italic>Pr (<jats:bold>5\u2009a<\/jats:bold>), Cy (<jats:bold>5\u2009b<\/jats:bold>)) were prepared from compounds <jats:bold>3\u2009a<\/jats:bold> and <jats:bold>3\u2009b<\/jats:bold> by silyl deprotection with TBAF and subsequent acidification of the intermediate salts [Re(H)(NO)(PR<jats:sub>3<\/jats:sub>)(C<jats:sub>5<\/jats:sub>H<jats:sub>4<\/jats:sub>O)][NBu<jats:sub>4<\/jats:sub>] (R=<jats:italic>i<\/jats:italic>Pr (<jats:bold>4\u2009a<\/jats:bold>), Cy (<jats:bold>4\u2009b<\/jats:bold>)) with NH<jats:sub>4<\/jats:sub>Br. In nonpolar solvents, compounds <jats:bold>5\u2009a<\/jats:bold> and <jats:bold>5\u2009b<\/jats:bold> formed an equilibrium with the isomerized <jats:italic>trans<\/jats:italic>\u2010dihydride cyclopentadienone species [Re(H)<jats:sub>2<\/jats:sub>(NO)(PR<jats:sub>3<\/jats:sub>)(C<jats:sub>5<\/jats:sub>H<jats:sub>4<\/jats:sub>O)] (<jats:bold>6\u2009a,b<\/jats:bold>). Deuterium\u2010labeling studies of compounds <jats:bold>5\u2009a<\/jats:bold> and <jats:bold>5\u2009b<\/jats:bold> with D<jats:sub>2<\/jats:sub> and D<jats:sub>2<\/jats:sub>O showed H\/D exchange at the H<jats:sub>Re<\/jats:sub> and H<jats:sub>O<\/jats:sub> positions. Compounds <jats:bold>5\u2009a<\/jats:bold> and <jats:bold>5\u2009b<\/jats:bold> were active catalysts in the transfer hydrogenation reactions of ketones and imines with 2\u2010propanol as both the solvent and H<jats:sub>2<\/jats:sub> source. The mechanism of the transfer hydrogenation and isomerization reactions was supported by DFT calculations, which suggested a secondary\u2010coordination\u2010sphere mechanism for the transfer hydrogenation of ketones.<\/jats:p>","DOI":"10.1002\/chem.201103685","type":"journal-article","created":{"date-parts":[[2012,3,27]],"date-time":"2012-03-27T18:09:19Z","timestamp":1332871759000},"page":"5701-5714","source":"Crossref","is-referenced-by-count":49,"title":["Bifunctional Rhenium Complexes for the Catalytic Transfer\u2010Hydrogenation Reactions of Ketones and 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