Bis(phosphinimino)methanide rare earth amides: Synthesis, structure, and catalysis of hydroamination/cyclization, hydrosilylation, and sequential hydroamination/hydrosilylation

Marcus Rastätter, Agustino, Peter W. Roesky

Research output: Contribution to journalArticlepeer-review

134 Citations (Scopus)

Abstract

A series of yttrium and lanthanide amido complexes [Ln{N-(SiHMe 2)2}2{CH(PPh2NSiMe3) 2}] (Ln = Y, La, Sm, Ho, Lu) were synthesized by three different pathways. The title compounds can be obtained either from [Ln{N(SiHMe 2)2}3(thf)2] and [CH 2(PPh2NSiMe3)2] or from KN-(SiHMe2)2 and [Ln(CH(PPh2NSiMe 3)2}-Cl2]2, while in a third approach the lanthanum compound was synthesized in a one-pot reaction starting from K{CH(PPh2NSiMe3)2}, LaCl3, and KN-(SiHMe2)2. All the complexes have been characterized by single-crystal X-ray diffraction. The new complexes, [Ln{N(SiHMe 2)2}2{CH(PPh2NSiMe3) 2}], were used as catalysts for hydroamination/cyclization and hydrosilylation reactions. A clear dependence of the reaction rate on the ionic radius of the center metal was observed, showing the lanthanum compound to be the most active one in both reactions. Furthermore, a combination of both reactions - a sequential hydroamination/hydrosilylation reaction - was also investigated.

Original languageEnglish
Pages (from-to)3606-3616
Number of pages11
JournalChemistry - A European Journal
Volume13
Issue number13
DOIs
Publication statusPublished - 21 Jun 2007

Keywords

  • Catalysis
  • Hydroamination
  • Hydrosilylation
  • N,P ligands
  • Rare earth metals

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