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Cation distributions within a cluster framework. Synthesis and structure of the carbon- and boron-centered zirconium cluster compounds KZr/sub 6/Cl/sub 15/C and CsKZr/sub 6/Cl/sub 15/B

Journal Article · · J. Am. Chem. Soc.; (United States)
DOI:https://doi.org/10.1021/ja00250a015· OSTI ID:6336002

The structures of the isotypic KZr/sub 6/Cl/sub 15/C and CsKZr/sub 6/Cl/sub 15/B have been established by single-crystal X-ray diffraction in space group Pmma, Z = 4 (R = 3.1, 3.9%, R/sub w/ = 3.2, 3.6%, respectively). These contain a matrix of Z-centered Zr/sub 6/Cl/sub 12/Z clusters linked together by trans-chlorine atoms to form separate linear and zigzag chains that are interconnected into a three-dimensional network by four additional bridging chlorides. This (Zr/sub 6/Cl/sub 12/Z)Cl/sub 6/2/ framework affords three types of chloride environments for the cations, a smaller one (a) of ten-coordination occupied by potassium or rubidium and a pair of larger sites (b) with lower multiplicity that are utilized by cesium etc. The two b-type metal sites exhibit (1) an elongated square-pyramidal environment which, for the matrix studied, leaves the cesium closer to four-coordinate and (2) a more distorted 6 + 2 position of 2/m symmetry. Some evident cation disorder especially in the b(2) site and a possible small distortion of the anion matrix are noted. Compounds of this type are made by the reaction of stoichiometric amounts of ZrCl/sub 4/ and Zr with C, B, or ZrNCl and the appropriate MCl in welded Ta containers at 850/sup 0/C. These reactions give, according to Guinier powder diffraction, > 95% yields of KZr/sub 6/Cl/sub 15/Z, Z = C or N, with occupancy of cation site a, the isotopic (Cs or Rb)Zr/sub 6/Cl/sub 15/C utilizing site b, and (CsK, Rb/sub 2/, or CsRB)Zr/sub 6/Cl/sub 15/B with a and b site occupancy. All but the nitride involve 14 cluster-bonding electrons, the most preferred state according to the MO scheme.

Research Organization:
Iowa State Univ., Ames
OSTI ID:
6336002
Journal Information:
J. Am. Chem. Soc.; (United States), Journal Name: J. Am. Chem. Soc.; (United States) Vol. 109:16; ISSN JACSA
Country of Publication:
United States
Language:
English