NDLI: Neutral ligand induced methane elimination from rare-earth metal tetramethylaluminates up to the six-coordinate carbide state

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Neutral ligand induced methane elimination from rare-earth metal tetramethylaluminates up to the six-coordinate carbide state

Content Provider	Royal Society of Chemistry (RSC)
Author	Berger, Raphael J. F. Stammler, Hans-Georg Venugopal, Ajay Neumann, Beate Mitzel, Norbert W. Kamps, Ina Willner, Alexander Mix, Andreas Bojer, Daniel
Copyright Year	2009
Abstract	The reaction of 1,3,5-trimethyl-1,3,5-triazacyclohexane (TMTAC) with [La{Al(CH3)4}3] resulted in C–H activation, leading to the formation of [(TMTAC)La{Al(CH3)4}{(μ3-CH2)[Al(CH3)2(μ2-CH3)]2}] (1) containing a bis(aluminate) dianion and subsequent extrusion of methane. A similar reaction with [Y{Al(CH3)4}3] led to the formation of CH4, [TMTAC{Al(CH3)3}2] (2) and {[(TMTAC)Y][Y2(μ2-CH3)][{(μ6-C)[Al(μ2-CH3)2(CH3)]3}{(μ3-CH2)(μ2-CH3)Al(CH3)2}2] (3), containing a six-coordinate carbide ion and two [CH2Al(CH3)3]2− anions. Compound 3 is a product of multiple C–H activation. This reaction was monitored by in situ1H NMR spectroscopy. The analogous reaction with [Sm{Al(CH3)4}3] led to the formation of 2, of [(TMTAC)Sm{(μ2-CH3)(CH3)2Al}2{(μ3-CH2)2Al(CH3)2}2] (4), which contains a tris(aluminate) trianion, and [{(TMTAC)Sm}{Sm2(μ2-CH3)}{(μ6-C)[Al(μ2-CH3)2(CH3)]3}{(μ3-CH2)(μ2-CH3)Al(CH3)2}2] (5), which is isostructural to 3. The products were characterised by elemental analyses (except 4, 5), 1 by multinuclear NMR spectroscopy and compounds 1, 2, 3, 4 and 5 by X-ray crystallography. Quantumchemical calculations were undertaken to support the crystallographic data analysis and confirm the structure of 3 and to compare it with an analogous compound where the central six-coordinate carbon has been replaced by oxygen. The investigations point to a mechanism of sterically induced condensation of [Al(CH3)4]−groups in close proximity in the coordination spheres of the rare-earth metal atoms, which is dependent on the size of these metal atoms.
Starting Page	5755
Ending Page	5765
Page Count	11
File Format	HTM / HTML PDF
ISSN	14779226
Volume Number	0
Issue Number	29
Journal	Dalton Transactions
DOI	10.1039/b905271b
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Carbon\u2013hydrogen bond activation Aluminate Methane Ion Nuclear magnetic resonance spectroscopy Elemental analysis 4 (Plain White T's song) X-ray crystallography Carbon Oxygen Rare earth element
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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