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Nitrene transfer to trimethylphosphine from citionic tungsten tosylnitrene complexes [Tp{prime}(CO){sub 2}W(NTs)][X]

Journal Article · · Inorganic Chemistry
; ; ;  [1]
  1. Univ. of North Carolina, Chapel Hill, NC (United States)

Reaction of Tp{prime}(CO){sub 3}WH(Tp{prime}=hydridotris(3.5-dimethyl-1-pyrazolyl)borate) with tosyl azide in THF at reflux affords the amido complex Tp{prime}(CO){sub 2}W(N(H)Ts) (1). Crystals of 1 are monoclinic, space group P2{sub 1}/n, with cell parameters a = 12.4855(11) A, b=20.5976(16){Angstrom}, c= 12.7311(11){Angstrom}, {beta}=96.510(10){degrees}, V=3253.0(5) {Angstrom}{sup 3}, and D{sub calcd}=1.591 g cm{sup {minus}3} for Z = 4. Least-squares refinement led to final R and R{sub w} values of 0.038 and 0.046, respectively. Complex 1 undergoes oxidation by silver triflate or iodine to give the imido complexes [Tp{prime}-(CO){sub 2}W(NTs)]X (X=OTf, 2a; X=I{sub 3},2b). The single crystal X-ray structure of 2b is also reported (orthorhombic, space group Pcab, a= 15.1764(16) {Angstrom}, b = 16.8890(14) {Angstrom}, c=26l909(3) {Angstrom}, V=6897.2(13) {Angstrom}{sup 3}, and D{sub calcd}= 2.094 g cm{sup {minus}3} for Z=8; R=0.044, R{sub 2}=0.052). The cationic nitrene complex 2 reacts with LiBH{sub 4} to regenerate the amido compound 1. Addition of trimethylphosphine to solutions of 2 leads to the formation of three species the phosphinimine TsN=PMe3 (3) and two tungsten complexes, [Tp{prime}(CO){sub 2}W(PMe{sub 3}){sub 2}][X](X = OTf, 4a; X=I{sub 3}, 4b) and [Tp{prime}(CO)(PMe{sub 3})W(NTs)][X] (X=OTf, 5a; X=I{sub 3}, 5b). Complex 5b undergoes substitution by iodide to produce the tungsten monocarbonyl Tp{prime}(CO)IW(NTs) (6).

Sponsoring Organization:
USDOE
DOE Contract Number:
FG05-85ER13430
OSTI ID:
417626
Journal Information:
Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 26 Vol. 33; ISSN 0020-1669; ISSN INOCAJ
Country of Publication:
United States
Language:
English

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