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Comparative study of fluxional processes at two different classes of eight-coordinate rhenium(V) polyhydride complexes
Two different structural types of dodecahedral rhenium(V) tetrahydride complexes were identified as capable of providing insight into a pseudorotational exchange of ligands at such complexes. One type of complex afforded an inequivalent set of NMR-active phosphorus atoms that occupy B sites in the rhenium coordination sphere along with four hydride ligands in the dodecahedral A sites. A second type of complex afforded the potential to inhibit the pseudorotational exchange of ligands at such complexes due to the presence of a chelating bidentate ligand. A pair of each type of complexes were studied by variable temperature NMR measurements and simulation of those measurements. The first type of complex exhibited pseudorotation of both the A site hydride ligands and the B site triphenylphosphine ligands. The first type of complexes also exhibited a pairwise exchange of the two inequivalent hydride ligands on the complexes. The second type of complex did not exhibit pseudorotational exchange of the A site hydride ligands, presumably due to the chelating bidentate ligand bound to rhenium. Instead, the A site hydride ligands of the second type of complex exhibited only exchange with the single B site hydride ligand through either a pairwise or a turnstile type of mechanism. Neither type of complex exhibited any direct intermolecular exchange of protons from the hydride ligand set with adventitious water from the solvent matrix. The value of Delta G(240)(double dagger) for each of the identified fluxional processes was close to 12 kcal/mol. The values of Delta S-double dagger for each fluxional process suggest that none of the processes are dissociative in nature.
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