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Synthesis, structural characterization, and electrochemistry of (1)Metallocenophane complexes, (Si(alkyl)/sub 2/(C/sub 5/H/sub 4/)/sub 2/)MCl/sub 2/, M = Ti, Zr

Journal Article · · Inorg. Chem.; (United States)
DOI:https://doi.org/10.1021/ic00210a015· OSTI ID:5826091

A series of modified metallocene dichloride compounds, (SiR/sub 2/(C/sub 5/H/sub 4/)/sub 2/)MCl/sub 2/ (M = Ti, R = CH/sub 3/; M = Zr, R = CH/sub 3/, C/sub 2/H/sub 5/, n-C/sub 3/H/sub 7/), have been prepared to evaluate the presence of a dialkylsilyl bridge on their electrochemical behavior. The compounds have been characterized by elemental analysis and /sup 1/H and /sup 13/C NMR, and the molecular structures of (Si(CH/sub 3/)/sub 2/(C/sub 5/H/sub 4/)/sub 2/)MCl/sub 2/, M = Ti, Zr, have been determined by X-ray diffraction methods. The /sup 13/C NMR resonance of the bridgehead carbons is consistently located substantially upfield from the corresponding resonances for the proximal and distal carbons of the rings in these compounds. Cyclic voltammetric measurements have shown that these (1)metallocenophane dichlorides exhibit only one one-electron reversible reduction in THF within a scan range of +1.0 to -3.0 V vs. SCE. Complementary EPR studies were conducted to identify and monitor the stability of the paramagnetic species generated during the electrochemical reduction of (Si(CH/sub 3/)/sub 2/(C/sub 5/H/sub 4/)/sub 2/)TiCl/sub 2/ and the sodium naphthalide reduction of (Si(CH/sub 3/)/sub 2/(C/sub 5/H/sub 4/)/sub 2/)MCl/sub 2/, M = Ti, Zr. These reduction processes proceed similarly with the formation of only one paramagnetic product, (Si(CH/sub 3/)/sub 2/(C/sub 5/H/sub 4/)/sub 2/)MCl/sub 2//sup -/. The compounds (Si(CH/sub 3/)/sub 2/(C/sub 5/H/sub 4/)/sub 2/)MCl/sub 2/, M = Ti, Zr, similarly crystallize in a monoclinic unit cell of C2/c symmetry with the following refined lattice parameters: for M = Ti, a = 13.309 (5) A, b = 9.871 (2) a, c = 13.337 (4) A, ..beta.. = 132.79 (1)/sup 0/, V = 1285.8 (7) A/sup 3/, and rho/sub calcd/ = 1.576 g/cm/sup 3/; for M = Zr, a = 13.391 (3) A, b = 9.965 (2) A, c = 10.922 (3) A, ..beta.. = 113.37 (2) A, V = 1337.8 (5) A/sup 3/, and rho/sub calcd/ = 1.730 g/cm/sup 3/. 44 references, 6 figures, 7 tables.

Research Organization:
West Virginia Univ., Morgantown
OSTI ID:
5826091
Journal Information:
Inorg. Chem.; (United States), Journal Name: Inorg. Chem.; (United States) Vol. 24:16; ISSN INOCA
Country of Publication:
United States
Language:
English