期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 133, 期 23, 页码 8826-8829出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja201989c
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- University of Bristol
The cationic zirconocene phosphinoaryloxide complexes [Cp2ZrOC6H4P(t-Bu)(2)] [B(C6F5)(4)] (3) and [Cp*2ZrOC6H4P(t-Bu)(2)][B(C6F5)(4)] (4) were synthesized by the reaction of Cp2ZrMe2 or Cp*2ZrMe2 with 2-(diphenyl-phosphino)phenol followed by protonation with [2,6-di-tert-butylpyridinium] [B(C6F5)(4)]. Compound 3 exhibits a Zr-P bond, whereas the bulkier Cp* derivative 4 was isolated as a chlorobenzene adduct without this Zr-P interaction. These compounds can be described as transition-metal-containing versions of linked frustrated Lewis pairs (FLPs), and treatment of 4 with H-2 under mild conditions cleaved H-2 in a fashion analogous to that for main-group FLPs. Their reactivity in amine borane dehydrogenation also mimics that of main-group FLPs, and they dehydrogenate a range of amine borane adducts. However, in contrast to main-group FLPs, 3 and 4 achieve this transformation in a catalytic rather than stoichiometric sense, with rates superior to those for previous high-valent catalysts.
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