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Issue 24, 2018
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Dinitrogen functionalization at a ditantalum center. Balancing N2 displacement and N2 functionalization in the reaction of coordinated N2 with CS2

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Abstract

The reaction of carbon disulfide (CS2) with the side-on end-on dinitrogen complex ([NPNSi]Ta)2(μ–η12-N2)(μ-H)2 (1) (where [NPNSi] = [PhP(CH2SiMe2NPh)2]) has been studied and shown to generate two products, the ratio of which depends on the concentration of added carbon disulfide. At high concentrations of CS2, N–N bond cleavage and functionalization occur to generate a ditantalum complex with an isothiocyanato ligand N-bound to Ta along with bridging sulfido and nitrido moieties. At lower concentrations of CS2, less dinitrogen functionalization is observed; instead, N2 is displaced and the CS2 molecule is completely disassembled to generate a ditantalum derivative with bridging methylene and two sulfide moieties. Kinetic and DFT studies have been performed and provide clues about the product ratio and mechanistic information and shed light on why N2 functionalization is challenging.

Graphical abstract: Dinitrogen functionalization at a ditantalum center. Balancing N2 displacement and N2 functionalization in the reaction of coordinated N2 with CS2

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Publication details

The article was received on 23 Apr 2018, accepted on 25 May 2018 and first published on 31 May 2018


Article type: Paper
DOI: 10.1039/C8DT01615A
Citation: Dalton Trans., 2018,47, 7983-7991
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    Dinitrogen functionalization at a ditantalum center. Balancing N2 displacement and N2 functionalization in the reaction of coordinated N2 with CS2

    R. J. Burford, L. Castro, L. Maron, J. E. Hein and M. D. Fryzuk, Dalton Trans., 2018, 47, 7983
    DOI: 10.1039/C8DT01615A

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