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Tunable Binding of Dinitrogen to a Series of Heterobimetallic Hydride Complexes

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The reaction of [Ru(H)2(N2)2(PCy3)2] (1) with β-diketiminate stabilized hydrides of Al, Zn, and Mg generates a series of new heterobimetallic complexes with either H2 or N2 ligated to the ruthenium… Click to show full abstract

The reaction of [Ru(H)2(N2)2(PCy3)2] (1) with β-diketiminate stabilized hydrides of Al, Zn, and Mg generates a series of new heterobimetallic complexes with either H2 or N2 ligated to the ruthenium center. Changing the main-group fragment of the M·Ru-N2 (M = Al, Zn, Mg) complexes can subtly alter the degree of binding, and therefore activation, of the diatomic ligand, as evidenced by the νN≡N absorptions in the infrared data. Experimental and computational data rationalize this tunable binding; decreasing the electronegativity of the main group in the order Al > Zn > Mg infers greater ionic character of these M·Ru-N2 complexes, and this in turn results in greater destabilization of the frontier molecular orbitals of ruthenium and therefore greater Ru(4d) → π*(N2) back-donation.

Keywords: heterobimetallic hydride; binding dinitrogen; series heterobimetallic; series; tunable binding; dinitrogen series

Journal Title: Organometallics
Year Published: 2018

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