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Extra resources for Progress in Inorganic Chemistry: Bioinorganic Chemistry, Volume 38

Example text

Odd- and even-electron clusters have ground states with S 2 4 and S = 0, respectively, and higher spin states that are thermally occupied. Protein effects propagated to the Fe subsites are presumably largely if not completely responsible for subsite inequivalence. This statement rests on structural determinations of [4Fe-4SI2+ analogue clusters, the core configurations of which without exception closely approach tetragonal (&) symmetry. Thus there appears to be no intrinsic inequivalence in subsites.

Our approach, which originates with the considerations and experimentation of Stack (207), has as its basis the striking conformations of certain hexasubstituted benzenes shown in Fig. 18. These are two of a number of examples of this class of compounds prepared by MacNicol and co-workers (208-210). 5-Me2C6H3)6(210) possess the hahaha conformation, in which the substituents are arranged below and above the central ring in serial order. One large substituent presumably buttresses its neighbors to positions on opposite sides of the ring.

The spectrum of the PNstate is shown in Fig. 15, and contains three subsite quadrupole doublets, Fez+,D, and S. Spectral analysis has led to the conclusion that the DebyeWaller factors for the different cluster subsites do not have the same temperature dependence and that the intensity ratio of the Fe2+,D, and S subsites is better described as 4: 10:2 instead of 4: 12:2, as in earlier work. Parameters of the Fez+ doublet are consistent with those of a tetrahedral FeI'S, unit as in reduced rubredoxin, and may be considered to define the "unique" subsite.

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