Stability and Ligand Exchange Reactions of Chromium(IV) Carboxylato Complexes in Aqueous Solutions

Inorganic Chemistry

Volumn 36, Issue 24, 1997, Pages 5440-5448

  Codd, Rachel ^a   Lay, Peter A ^a   Levina, Aviva ^a  

^a UNIVERSITY OF SYDNEY   (Australia)

Author keywords

[No Author keywords available]

Indexed keywords

EID: 0001017299     PISSN: 00201669     EISSN: None     Source Type: Journal    
DOI: 10.1021/ic970834r     Document Type: Article

References (59)

1. The following abbreviations for the ligands were used in this work: hmba = 2-hydroxy-2-methylbutanoate(2-); edta = ethylenediamine-tetraacetate(4-); ehba = 2-ethyl-2-hydroxybutanoate(2-); mal = malonate (propanedioate(2-)); ox = oxalate (ethanedioate(2-)); pic = picolinate (2-pyridinecarboxylate(-)); qa = (-)-quinate ((1R,3R,4R,5R)-l,3,4,5-tetrahydroxycyclohexanecarboxylate(2-)); Lig = any of the above-mentioned ligands.
2. Larkworthy, L. F.; Nolan, K. B.; O'Brien, P. In Comprehensive Coordination Chemistry; Wilkinson, G.; Gillard, R. D.; McCleverty, J. A., Eds.; Pergamon Press: Oxford, U.K., 1987; Vol. 3, pp 699-969.
3. Gould, E. S. Coord. Chem. Rev. 1994, 135/136, 651-684 and references therein.
4. Ghosh, M. C.; Gould, E. S. Inorg. Chem. 1991, 30, 491-494.
5. (a) Krumpolc, M.; Roček, J. J. Am. Chem. Soc. 1978, 100, 145-153.
6. (b) Krumpolc, M.; Roček, J. J. Am. Chem. Soc. 1979, 101, 3206-3209.
7. Judd, R. J.; Hambley, T. W.; Lay, P. A. J. Chem. Soc., Dalton Trans. 1989, 2205-2210.
8. Fanchiang, Y.-T.; Bose, R. N.; Gelerinter, E.; Gould, E. S. Inorg. Chem. 1985, 24, 4679-4684.
9. Ghosh, M. C.; Gelerinter, E.; Gould, E. S. Inorg. Chem. 1992, 31, 702-705.
10. (a) Scott, S. L.; Bakac, A.; Espenson, J. H. J. Am. Chem. Soc. 1992, 114, 4205-4213.
11. (b) Bakac, A.; Espenson, J. H. Acc. Chem. Res. 1993, 26, 519-523.
12. Bose, R. N.; Moghaddas, S.; Gelerinter, E. Inorg. Chem. 1992, 31, 1987-1994.
13. Barr-David, G.; Hambley, T.; Irwin, J. A.; Judd, R. J.; Lay, P. A.; Martin, B. D.; Bramley, R.; Dixon, N. E.; Hendry, P.; Ji, J. Y.; Baker, R. S. U.; Bonin, A. M. Inorg. Chem. 1992, 31, 4906-4908.
14. (a) Sugden, K. D.; Wetterhahn, K. E., J. Am. Chem. Soc. 1996, 118, 10811-10818.
15. (b) Stearns, D. M.; Wetterhahn, K. E. Chem. Res. Toxicol. 1997, 10, 271-278.
16. (a) Luo, H.; Lu, Y.; Shi, X.; Mao, Y.; Dalal, N. S. Ann. Clin. Lab. Sci. 1996, 26, 185-191.
17. (b) Luo, H.; Lu, Y.; Mao, Y.; Shi, X.; Dalal, N. S. J. Inorg. Biochem. 1996, 64, 25-35.
18. Farrell, R. P.; Judd, R. J.; Lay, P. A.; Dixon, N. E.; Baker, R. S. U.; Bonin, A. M. Chem. Res. Toxicol. 1989, 2, 227-229.
19. Dillon, C. T.; Lay, P. A.; Bonin, A. M.; Dixon, N. E.; Collins, T. J.; Kostka, K. L. Carcinogenesis 1993, 14, 1875-1880.
20. The lower pH values relate to the conditions in certain cellular organelles, lysosomes, that uptake and solubilize Cr compounds by phagocytosis and play an important role in genotoxicities of insoluble chromates: (a) Elias, Z.; Poirot, O.; Pezerat, H.; Suquet, H.; Schneider, O.; Danière, M. C.; Terzetti, F.; Baruthio, F.; Fournier, M.; Cavelier, C. Carcinogenesis 1989, 10, 2043-2052. (b) Cohen, M. D.; Costa, M. In Environmental and Occupational Medicine, 2nd ed.; Rom, W. N., Ed.; Little Brown and Co.: Boston, MA, 1992; pp 799-805.
21. The lower pH values relate to the conditions in certain cellular organelles, lysosomes, that uptake and solubilize Cr compounds by phagocytosis and play an important role in genotoxicities of insoluble chromates: (a) Elias, Z.; Poirot, O.; Pezerat, H.; Suquet, H.; Schneider, O.; Danière, M. C.; Terzetti, F.; Baruthio, F.; Fournier, M.; Cavelier, C. Carcinogenesis 1989, 10, 2043-2052. (b) Cohen, M. D.; Costa, M. In Environmental and Occupational Medicine, 2nd ed.; Rom, W. N., Ed.; Little Brown and Co.: Boston, MA, 1992; pp 799-805.
22. Ghosh, M. C.; Gould, E. S. J. Am. Chem. Soc. 1993, 115, 3167-3173.
23. Bose, R. N.; Fonkeng, B.; Barr-David, G.; Farrell, R. P.; Judd, R. J.; Lay, P. A.; Sangster, D. F. J. Am. Chem. Soc. 1996, 118, 7139-7144.
24. Ghosh, M. C.; Bose, R. N.; Gelerinter, E.; Gould, E. S. Inorg. Chem. 1992, 31, 1709-1713.
25. (a) Leonard, A.; Lauwerys, R. R. Mutat. Res. 1980, 75, 49-62.
26. (b) Leonard, A.; Lauwerys, R. R. Mutat. Res. 1980, 76, 227-239.
27. The "ligand acids" were checked for the absence of reducing impurities, as described in: Chandra, S. K.; Gelerinter, E.; Gould, E. S. Res. Chem. Intermed. 1996, 22, 43-52.
28. Codd, R.; Zhang, L.; Freeman, H. C.; Lay, P. A. To be submitted for publication.
29. De Meester, P.; Hodgson, D. J.; Freeman, H. C.; Moore, C. J. Inorg. Chem. 1977, 16, 1494-1498.
30. Palmer, W. G. Experimental Inorganic Chemistry; Cambridge University Press: Cambridge, U.K., 1954; p 319.
31. Skoog, D. A.; West, D. M.; Holler F. J. Fundamentals of Analytical Chemistry, 7th ed.; Saunders College Publishing: New York, 1996; pp 366-372.
32. King, P. J.; Maeder, M. Glint - Global Kinetic Analysis, Version 3.31; Applied Photophysics Ltd.: Leatherhead, U.K., 1993.
33. Lay, P. A.; Levina, A. Inorg. Chem. 1996, 35, 7709-7717.
34. The reaction times, providing quantitative yields of Cr(IV), were dependent on [Lig], pH, and temperature and were chosen from the kinetics of Cr(IV) formation.
35. 3).
36. Origin. Technical Graphics and Data Analysis for Windows, Version 4.1; Microcal Software Inc.: Northampton, MA, 1996.
37. Krumpolc, M.; Roček, J. Inorg. Chem. 1985, 24, 617-621.
38. Haupt, G. W. Natl. Bur. Stand. Circ. (U.S.) 1952, 48, 414-423.
39. Form, G. E.; Raper, E. S.; Oughtred, R. E.; Shearer, H. M. M. J. Chem. Soc., Chem. Commun. 1972, 945-946.
40. WIN-EPR, Version 921201; Bruker-Franzen Analytic GmbH: Bremen, Germany, 1996.
41. Hambley, T. W.; Judd, R. J.; Lay, P. A. Inorg. Chem. 1992, 31, 345-351.
42. (a) Chasteen, N. D. Struct. Bonding (Berlin) 1983, 53, 105-138.
43. (b) Codo, R.; Hambley, T. W.; Lay, P. A. Inorg. Chem. 1995, 34, 877-882.
44. EPR spectral data on the Cr(V) complexes have been published: Barr-David, G.; Bramley, R.; Brumby, S.; Charara, M.; Codd, R.; Farrell, R. P.; Hanson, G. R.; Irwin, J. A.; Ji, J.-Y.; Lay, P. A. J. Chem. Soc., Faraday Trans. 1995, 91, 1207-1216.
45. 2 in more acidic media (pH = 0-1.5). See: (a) Farrell, R. P.; Judd, R. J.; Lay, P. A.; Bramley, R.; Ji, J.-Y. Inorg. Chem. 1989, 28, 3403-3410. (b) Farrell, R. P. Ph.D. Thesis, University of Sydney, 1993.
46. 2 in more acidic media (pH = 0-1.5). See: (a) Farrell, R. P.; Judd, R. J.; Lay, P. A.; Bramley, R.; Ji, J.-Y. Inorg. Chem. 1989, 28, 3403-3410. (b) Farrell, R. P. Ph.D. Thesis, University of Sydney, 1993.
47. (a) Branca, M.; Dessí, A.; Kozlowski, H.; Micera, G.; Swiatek, J. J. Inorg. Biochem. 1990, 39, 217-226.
48. (b) Irwin, J. A. Unpublished results.
49. Ohashi, K.; Aramaki, M.; Kaise, M.; Yamamoto, K. Anal. Sci. 1989, 5, 73-77.
50. 7 of the system Cr(V) + V(IV) + ehba. This led to some misinterpretations of the kinetic data. Thus, the formation and decomposition of Cr(IV) (monitored at 490 nm) were assigned to three sequential steps. In fact, there are only two steps corresponding to the formation and decomposition of Cr(IV), respectively (as shown from absorbance changes at 560 nm, where the influence of [V(V)] is negligible). The third step observed at 490 nm corresponds to further transformations of V(V)-ehba.
51. 4.
52. This refers to the reactions in ehba, hmba, and qa buffers at pH = 2.5-4.5.
53. Electrochemical studies (Eckert, J. M.; Judd, R. J.; Lay, P. A. Inorg Chem. 1987, 26, 2191-2192) show that Cr(V) complexes are more powerful oxidants than Cr(VI) compounds.
54. (a) Mitewa, M.; Bontchev, P. R. Coord. Chem. Rev. 1985, 6, 241-272.
55. (b) Farrell, R. P.; Lay, P. A. Comments Inorg. Chem. 1992, 13, 133-175.
56. -1.9 (47) The effects of pH on the structures of Cr(V)-qa complexes in aqueous solutions have been studied in detail by EPR spectroscopy (Codd, R. Unpublished results).
57. The analysis of the reaction mixtures show that only Cr(III), not Cr(V) or Cr(VI), is present in the reaction mixtures after the decomposition of the Cr(IV)-qa complex at pH < 3. Thus, the ligand oxidation is the only significant pathway of Cr(IV)-qa decomposition under these conditions.
58. Dillon, C. T. Ph.D. Thesis, University of Sydney, 1995.
59. Liu, K. J.; Shi, X.; Jiang, J.; Goda, F.; Dalal, N.; Swartz, H. M. Ann. Clin. Lab. Sci. 1996, 26, 176-184.