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Experimental and Computational Studies on Quadruply Bonded Dimolybdenum Complexes with Terminal and Bridging Hydride
Marina Pérez-Jiménez1, Natalia Curado1, Celia Maya1
1Instituto de Investigaciones Químicas (IIQ), Departamento de Química Inorgánica and Centro de, Innovación en Química Avanzada (ORFEO-CINQA), Consejo Superior de Investigaciones Científicas (CSIC) and University of Sevilla, Avda. Américo Vespucio, 49, 41092, Sevilla, Spain.
Abstract:
This contribution focuses on complex [Mo2 (H)2 (μ-AdDipp2 )2 ] (1) and tetrahydrofuran and pyridine adducts [Mo2 (H)2 (μ-AdDipp2 )2 (L)2 ] (1⋅thf and 1⋅py), which contain a trans-(H)Mo≣Mo(H) core (AdDipp2 =HC(NDipp2 )2 ; Dipp=2,6-iPr2 C6 H3 ). Computational studies provide insights into the coordination and electronic characteristics of the central trans-Mo2 H2 unit of 1, with four-coordinate, fourteen-electron Mo atoms and ϵ-agostic interactions with Dipp methyl groups. Small size C- and N-donors give rise to related complexes 1⋅L but only one molecule of P-donors, for example, PMe3 , can bind to 1, causing one of the hydrides to form a three-centered, two-electron (3c-2e) Mo-H→Mo bond (2⋅PMe3 ). A DFT analysis of the terminal and bridging hydride coordination to the Mo≣Mo bond is also reported, along with reactivity studies of the Mo-H bonds of these complexes. Reactions investigated include oxidation of 1⋅thf by silver triflimidate, AgNTf2 , to afford a monohydride [Mo2 (μ-H)(μ-NTf2 )(μ-AdDipp2 )2 ] (4), with an O,O'-bridging triflimidate ligand.
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