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Insights into the decomposition pathway of a lutetium alkylamido complex via intramolecular C–H bond activation

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Knott, J. P., Hänninen, M. M., Rautiainen, M., Tuononen, H., & Hayes, P. G. (2017). Insights into the decomposition pathway of a lutetium alkylamido complex via intramolecular C–H bond activation. Journal of Organometallic Chemistry, 845, 135-143. doi:10.1016/j.jorganchem.2017.04.008
Published in
Journal of Organometallic Chemistry
Authors
Knott, Jackson P. |
Hänninen, Mikko M. |
Rautiainen, Mikko |
Tuononen, Heikki |
Hayes, Paul G.
Date
2017
Discipline
Epäorgaaninen ja analyyttinen kemia
Copyright
© 2017 Elsevier Ltd. This is a final draft version of an article whose final and definitive form has been published by Elsevier. Published in this repository with the kind permission of the publisher.

 
Synthesis, characterization and reaction chemistry of lutetium alkylamido LLu(CH2SiMe3)(NHCPh3) (2), L = 2,5-[Ph2P=N(4-iPrC6H4)]2N(C4H2)–, is reported. Complex 2 undergoes cyclometalation of the NHCPh3 ligand at elevated temperatures to produce the orthometalated complex LLu(κ2−N,C-(NHCPh2(C6H4))) (3) which converts to 0.5 equivalents of bis(amido) LLu(NHCPh3)2 (4) upon heating at 80 °C for 24 h. Reaction of complex 2 with 4-dimethylaminopyridine (DMAP) does not promote alkane elimination nor imido formation. A kinetic analysis of the thermal decomposition of complex 2, supported by deuterium labelling studies and computational analysis (PBE0/def2-TZVP/SDD(Lu)), indicate direct Csp2–H activation, rather than C–H addition across a transient LLu=NCPh3 species, occurs.
Publisher
Elsevier B.V.
ISSN Search the Publication Forum
0022-328X
Keywords
coordination complexes lutetium
DOI
https://doi.org/10.1016/j.jorganchem.2017.04.008
URI

http://urn.fi/URN:NBN:fi:jyu-201707213350

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