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1,1-digoldallylium complexes: diaurated allylic carbocations indicate new prospects of the coordination chemistry of carbon

Reacting (NHC)(cyclopropenyl)gold(I) complexes with cationic gold complexes [(IPr)AuX] afforded extremely reactive allylium-1,1-diido-bridged digold intermediates. We prove the existence and constitution of this structure with FT-ICR-MS/MS, NMR, and UV-vis-NIR experiments and isolated the nucleophil...

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Hauptverfasser: Mulks, Florian (VerfasserIn) , Antoni, Patrick W. (VerfasserIn) , Gross, Jürgen H. (VerfasserIn) , Graf, Jürgen (VerfasserIn) , Rominger, Frank (VerfasserIn) , Hashmi, A. Stephen K. (VerfasserIn)
Dokumenttyp: Article (Journal)
Sprache:Englisch
Veröffentlicht: [2019]
In: Journal of the American Chemical Society
Year: 2019, Jahrgang: 141, Heft: 11, Pages: 4687-4695
ISSN:1520-5126
DOI:10.1021/jacs.8b13395
Online-Zugang:Verlag, Volltext: https://doi.org/10.1021/jacs.8b13395
Volltext
Verfasserangaben:Florian F. Mulks, Patrick W. Antoni, Jürgen H. Gross, Jürgen Graf, Frank Rominger, and A. Stephen K. Hashmi (Organisch-Chemisches Institut, Heidelberg University)

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520 |a Reacting (NHC)(cyclopropenyl)gold(I) complexes with cationic gold complexes [(IPr)AuX] afforded extremely reactive allylium-1,1-diido-bridged digold intermediates. We prove the existence and constitution of this structure with FT-ICR-MS/MS, NMR, and UV-vis-NIR experiments and isolated the nucleophilic addition product [(Me)(Ph)(CCHC){Au(IPr)}2(SOMe2)]NTf2 with DMSO. Our computational investigation unveiled that the bonding situation of this μ-allylium-1,1-diido digold domain was best described as a three-center-four-electron bond with a π-backbond. The valence orbitals showed extreme delocalization and strong π-interactions between the three centers Au1-C1-Au2. The bridging carbon atom C1 was best described as trigonal planar sp-hybridized carbon in this structure. Excitation succeeded in UV-vis-NIR measurements with energies as low as near-IR radiation. 
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