A half-sandwich molybdenum(II) thiolate complex with a η 2 -MeCN ligand, Cp*Mo(1,2-Ph 2 PC 6 H 4 S)(η 2 -NCMe) (1(η 2 -NCMe)), was found to catalyze transfer hydrogenation of nitriles efficiently with ammonia borane (H 3 N•BH 3 ) at room temperature, producing primary amines. Through molybdenum-thiolate cooperation, the B−H bond of BH 3 is cleaved, affording a Mo(II)-H hydride (1H(BH 2 )) with the BH 2 moiety captured at the S−Mo unit. In the presence of NH 3 , 1H(BH 2 ) smoothly achieves the catalytic transfer hydrogenation of nitriles.

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