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Synthesis, spectroscopy, and structural characterization of five-coordinate, bis(aryldiazenido)technetium complexes and their protonation reactions. X-ray structure of (TcCl(PPh sub 3 ) sub 2 (NNC sub 6 H sub 4 Br) sub 2 )

Journal Article · · Inorganic Chemistry; (USA)
DOI:https://doi.org/10.1021/ic00319a013· OSTI ID:7108190
; ;  [1];  [2]
  1. Massachusetts Institute of Technology, Cambridge (USA)
  2. Harvard Medical School, Boston, MA (USA)

The reaction of (TcCl{sub 4}(PPh{sub 3}){sub 2}) with arylhydrazines in methanol yields (TcCl(PPh{sub 3}){sub 2}(NNPh){sub 2}) (1). Complex 1 displays trigonal-bipyramidal geometry with phosphine ligands occupying axial sites. The technetium-aryldiazenido moieties are nearly equivalent, with Tc-N-N bond angles of 166.2 (6) and 170.7 (7){degree} and multiple bonding throughout. The chloride ligand occupies the remaining equatorial coordination site. The addition of HCl(g) to complex 1 in methanol gives the neutral, six-coordinate hydrazido(2-) complex (TcCl{sub 2}(PPh{sub 3}){sub 2}(NNPh)(NNHPh)). The reaction of complex 1 with HBr(g) gives the doubly protonated, cationic species (TcBr{sub 2}(PPh{sub 3}){sub 2}(NNPh)(NHNHPh))(Br). The {sup 99}Tc NMR spectra for these species are presented, which suggest that the metals exhibit considerable Tc(V) character and that the formal oxidation states of {minus}1 and +1 are not accurate ddescriptions of the electron density on the technetium. The {sup 1}H NMR, mass, and electronic spectroscopic data are also presented for the various species, along with the crystal structure of the five-coordinate bis(aryldiazenido) precursor. Crystal data for C{sub 48}H{sub 38}N{sub 4}P{sub 2}ClBr{sub 2}Tc are presented.

OSTI ID:
7108190
Journal Information:
Inorganic Chemistry; (USA), Journal Name: Inorganic Chemistry; (USA) Vol. 28:20; ISSN 0020-1669; ISSN INOCA
Country of Publication:
United States
Language:
English