Imine Metathesis Catalyzed by a Silica-supported Hafnium Imido Complex

Maha A. Aljuhani, Samir Barman, Edy Abou-Hamad, Andrei Gurinov, Samy Ould-Chikh, Erjia Guan, Abdesslem Jedidi, Luigi Cavallo, Bruce C. Gates, Jeremie Pelletier, Jean-Marie Basset

Research output: Contribution to journalArticlepeer-review

9 Scopus citations

Abstract

ABSTRACT: Well-defined single-site silica-supported haf-niaaziridine complex [(≡Si-O-)Hf(η2-MeNCH2)(η1-NMe2)(η1-HNMe2)] was prepared using surface organometallic chemistry. Upon thermal treatment under high vacuum, the grafted spe-cies was converted into an unprecedented hafnium imido, bis-amido, complex [(≡Si-O-)Hf(=NMe)(η1-NMe2)]. The surface complexes were characterized by elemental analysis and the following spectroscopic techniques: infrared, solid-state single and multiple quantum NMR, advanced DNP-SENS, and ex-tended X-ray absorption fine structure. [(≡Si-O-)Hf(=NMe)(η1-NMe2)] catalyzed imine metathesis under mild conditions, and characterization of the reactivity showed that the imido ex-change with N-(4-phenylbenzylidene)benzylamine yielded [(≡Si-O-)Hf (η2-NMeNCH2ArCH2) (η1-NMe2)], demonstrating a kind of 2+2 mechanism involving the imine and the imido, proposed reaction mechanism is also supported by DFT calculations.
Original languageEnglish (US)
Pages (from-to)9440-9446
Number of pages7
JournalACS Catalysis
Volume8
Issue number10
DOIs
StatePublished - Sep 4 2018

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