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This paper outlines the generation of the transient monomeric imido complexes Cp2Zr= NR (la-e), their successful trapping with unsaturated organic molecules and dative ligands, and their use in activating C—H bonds. The generation of Cp2Zr= NR has beenaccomplished by thermolysis of the alkyl amides Cp2Zr (NHR)(R0 (2a-d) and bis (amides) Cp2Zr (NHR) 2 (3a-c) via «-abstraction of alkane and amine, respectively. The imido intermediate la, generated from alkyl amide 2a (R= 4-tert-butylphenyl, R'= Me) in THF, resulted in the formation of the bridging imido dimer 4a in 70% yield. In contrast, the generation of intermediates lb-d (lb R= tert-Bu; lc R= 2, 6-dimethylphenyl; Id R= Si (CMe3) Me2) undersimilar conditions furnished the monomeric imido THF complexes 5b-d in 71, 69, and 72% yields. Imido dimer 4a and monomer 5b were characterized crystallographically. The THF ligands of 5b-d are weakly bound …