This paper reports the synthesis, structure, and properties of a series of PNP pincer complexes of osmium OsH3Cl[HN(C2H4PiPr2)2] (1), OsH3[N(C2H4PiPr2)2] (2), OsH4[HN(C2H4PiPr2)2] (3), and OsH2(PMe3)[HN(C2H4PiPr2)2] (4). The tetrahydride 3 operates as an efficient catalyst at 0.1 mol% loading for the reactions of amination and dehydrogenative coupling of primary alcohols, producing secondary amines and symmetrical esters, respectively. The catalyst 3 is distinguished by outstanding stability, and it can be used in an aqueous environment at temperatures as high as 200 °C.
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