The addition of CH3CHO to a chloroform
solution of H(μ-H)Os3(CO)10(NH3) affords the new H(μ-H)Os3(CO)10(HNCHCH3) derivative where the imine
ligand occupies a terminal position. The stereochemistry
of the adduct appears to be determined by the occurrence
of an unconventional hydrogen-bond interaction involving the N−H moiety and the terminal hydride.
Imine ligands terminally bound to triosmium clusters have been prepared by the reaction of Os 3 (µ-H) 2 -(CO) 10 with NH 3 and a keto or aldhehydic substrate. However reactions in nonpolar solvents yield only one of the two possible isomers. In contrast, reactions in polar solvents, such as methanol, yield both isomers. Experimental methods are described that clearly demonstrate that the overall stereochemistry of the resulting complexes is dependent upon the competition between intraand intermolecular hydrogen-bonding interactions. The isomers have been unambiguously assigned using 15 N and 13 C labeling as well as T 1 measurements.
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