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Issue 6, 2021
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σ or π? Bonding interactions in a series of rhenium metallotetrylenes

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Abstract

Salt metathesis reactions between a low-valent rhenium(I) complex, Na[Re(η5-Cp)(BDI)] (BDI = N,N′-bis(2,6-diisopropylphenyl)-3,5-dimethyl-β-diketiminate), and a series of amidinate-supported tetrylenes of the form ECl[PhC(NtBu)2] (E = Si, Ge, Sn) led to rhenium metallotetrylenes Re(E[PhC(NtBu)2])(η5-Cp)(BDI) (E = Si (1a), Ge (2), Sn (4)) with varying extents of Re–E multiple bonding. Whereas the rhenium–stannylene 4 adopts a σ-metallotetrylene arrangement featuring a Re–E single bond, the rhenium–silylene (1a) and –germylene (2) both engage in π-interactions to form short Re–E multiple bonds. Temperature was found to play a crucial role in reactions between Na[Re(η5-Cp)(BDI)] and SiCl[PhC(NtBu)2], as manipulation of reaction conditions led to isolation of an unusual rhenium–silane, (BDI)Re(μ-η51-C5H4)(SiH[PhC(NtBu)2]) (1b) and a dinitrogen bridged rhenium–silylene, (η5-Cp)(BDI)Re(μ-N2)Si[PhC(NtBu)2] (1c), in addition to 1a. Finally, the reaction of Na[Re(η5-Cp)(BDI)] with GeCl2·dioxane led to a rare μ2-tetrelido complex, μ2-Ge[Re(η5-Cp)(BDI)]2 (3). Bonding interactions within these complexes are discussed through the lens of various spectroscopic, structural, and computational investigations.

Graphical abstract: σ or π? Bonding interactions in a series of rhenium metallotetrylenes

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Article information


Submitted
14 Jan 2021
Accepted
14 Jan 2021
First published
22 Jan 2021

Dalton Trans., 2021,50, 2083-2092
Article type
Paper

σ or π? Bonding interactions in a series of rhenium metallotetrylenes

E. T. Ouellette, A. Carpentier, I. Joseph Brackbill, T. D. Lohrey, I. Douair, L. Maron, R. G. Bergman and J. Arnold, Dalton Trans., 2021, 50, 2083
DOI: 10.1039/D1DT00129A

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