A triad of d10 cobalt dihydrogen complexes was synthesized by utilizing Lewis acidic group 13 metalloligands, M[N((o-C6H4)NCH2PiPr2)3], where M = Al, Ga, and In. These complexes have formal Co(-I) oxidation states, representing the only coordination complexes in which dihydrogen is bound to a subvalent transition metal center. Single-crystal X-ray diffraction and NMR studies support the assignment of these complexes as nonclassical dihydrogen adducts of Co(-I).
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The authors thank Dr. Laura Clouston and Ryan Cammarota for synthetic assistance, Dr. Vic Young, Jr. for crystallographic expertise, Dr. Letitia Yao for help in NMR experiments, and Prof. Robert Morris (U of Toronto) and Prof. Laura Gagliardi for insightful discussions. M.V.V. thanks the National Science Foundation for a graduate research fellowship. J.X. thanks the Minnesota Supercomputing Institute (U of M) for computational resources.