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Properties and reactivities of pentadentate ethylenediaminetetraacetate complexes of ruthenium(III) and -(II)

Journal Article · · Inorg. Chem.; (United States)
DOI:https://doi.org/10.1021/ic50197a047· OSTI ID:5939126
The reaction of the pentadentate edta complex of ruthenium(III) with various entering ligands L has been studied as a function of pH, temperature, and L at 0.2 M ionic strength in aqueous solution. Over the pH range 0.8 to 8.5, the species Ru/sup III/(edta)H/sub 2/O/sup -/ is the sole form reactive in the substitution processes. Both forward (k/sub 1/) and reverse (k/sub -1/) rate constants Ru(edta)H/sub 2/O/sup -/ + L in equilibrium (k/sub 1/,k/sub -1/) Ru(edta)L/sup -/ + H/sub 2/O have been determined, as well as activation parameters for the complexation (k/sub 1/) process (L, k/sub 1/ in M/sup -1/s/sup -1/ (25/sup 0/C), k/sub -1/ in s/sup -1/ (25/sup 0/C), ..delta..H/sub 1//sup +/ in kcal mol/sup -1/, ..delta..S/sub 1//sup +/ in cal deg/sup -1/ mol/sup -1/): acetonitrile, 30 +- 7, 3.2 +- 0.2, 8.3 +- 0.5, -24 +- 4; thiocyanate, 270 +- 20, 0.5 +- 0.1, 8.9 +- 0.5, -18 +- 3; pyridine, 6300 +- 500, 0.061 +- 0.002; isonicotinamide, 8300 +- 600, 0.7 +- 0.2, 6.6 +- 0.5, -19 +- 3; pyrazine, 20,000 +- 1000, 2.0 +- 0.5, 5.7 +- 0.5, -20 +- 3. Forward rate constants for the analogous substitution reaction for Ru/sup II/(edta) H/sub 2/O/sup 2 -/ (25/sup 0/C, 0.2 M ionic strength) are as follows: thiocyanate, 2.7 +- 0.2 M/sup -1/s/sup -1/; acetonitrile, 13 +- 1 M/sup -1/s/sup -1/; isonicotinamide, 30 +- 15 M/sup -1/s/sup -1/. The substitution reactions of Ru/sup III/(edta)H/sub 2/O/sup -/ proceed by an associative mechanism, while those of Ru/sup II/(edta)H/sub 2/O/sup 2/- appear to be dissociative in nature. Spectra and reduction potentials for the Ru(edta)L/sup -/2-/ complexes are reported. 4 figures, 11 tables.
Research Organization:
Brookhaven National Lab., Upton, NY
OSTI ID:
5939126
Journal Information:
Inorg. Chem.; (United States), Journal Name: Inorg. Chem.; (United States) Vol. 18:7; ISSN INOCA
Country of Publication:
United States
Language:
English