Supramolecular Conformational Effects in the Electrocatalytic Properties of Electrostatic Assembled Films of Meso(3- and 4-Pyridyl) Isomers of Tetraruthenated Porphyrins
Keywords:
Supramolecular chemistry, metalloporphyrins, electrostatic assembled films, electrocatalysis, electrochemistry, mass spectrometryAbstract
Abstract. Meso(3- e4-pyridyl)porphyrins coordinated to four [Ru(bipy)2Cl]+ complexes, M(3-TRPyP) or M(4-TRPyP), where M=2H+ and Zn2+, have been obtained and characterized by electrochemistry, spectroscopy and mass spectrometry. Layer-by-layer electrostatic assembled films with tetrasulfonated phthalocyaninatecuprate(II) anion, CuTSPc, displayed distinct electrocatalytic activity towards sulfite
and nitrite oxidation. In general, the films derived from the M(4-TRPyP) isomers are more effective for the oxidation of nitrite, whereas those containing the M(3-TRPyP) isomers are more efficient for the oxidation of sulfite. The results demonstrated the influence of molecular geometry on the active sites of porphyrinic nanomaterials, enhancing the electron-transfer process in the M(3-TRPyP) derivative. This effect results from changes in the chemical environment around the active sites, induced by the contrasting molecular packing interactions with CuTSPc.
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References
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3. Wojaczynski, J.; Latos-Grazynski, L.; Coord. Chem. Rev. 2000, 204, 113.
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6. Nakash, M.; Clyde-Watson, Z.; Feeder, N.; Teat, S. J.; Sanders, J. K. M.; Chem. Eur. J. 2000, 6, 2112.
7. Toma, H. E.; Araki, K.; Coord. Chem. Rev. 2000, 196, 307.
8. Kadish, K. M.; Smith, K. M.; Guilard, R.; The Porphyrin Handbook, Academic Press: Amsterdam, 2003, vols. 7, 8, 11.
9. Murakami, Y.; Kikuchi, J.; Hisaeda, Y.; Hayashida, O.; Chem. Rev. 1996, 96, 721.
10. Meunier, B.; Chem. Rev. 1992, 92, 1411.
11. Barley, M. H.; Takeuchi, K. J.; Meyer, T. J.; J. Am. Chem. Soc. 1986, 108, 5876.
12. Cheng, S. H.; Su, Y. O.; Inorg. Chem. 1994, 33, 5847.
13. Hayon, J.; Raveh, A.; Bettelheim, A.; J. Electroanal. Chem. 1993, 359, 209.
14. Pang, D. W.; Wang, Z. L.; J. Electroanal. Chem. 1993, 358, 235.
15. Chen, S. M.; Chen, S. V.; Electrochim. Acta 2003, 48, 4049.
16. Ruhlmann, L.; Genet, G.; J. Electroanal. Chem. 2004, 568, 315.
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18. Lei, H. P.; Trofimova, N. S.; Ikeda, O.; Chem. Lett. 2003, 32, 610.
19. Collman, J. P.; Fu, L.; Acc. Chem Res. 1999, 32, 455.
20. Meunier, B.; Visser, S. P.; Shaik, S.; Chem. Rev. 2004, 104, 3947.
21. Shi, C. N.; Anson, F. C.; Inorg. Chem. 1992, 31, 5078.
22. Anson, F. C.; Shi, C. N.; Steiger, B.; Acc. Chem. Res. 1997, 30, 437.
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26. Casero, E.; Losada, J.; Pariente, F.; Lorenzo, E.; Talanta 2003, 61, 61.
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28. Azevedo, C. M. N.; Araki, K.; Angnes, L.; Toma, H. E.; Electroanal. 1998, 10, 467.
29. Araki, K.; Wagner, M. J.; Wringhton, M. S.; Langmuir 1996, 12, 5393.
30. Bedioui, F.; Villeneuve, N.; Electroanalysis 2003, 15, 5.
31. da Rocha, J. R. C.; Angnes, L.; Bertotti, M.; Araki, K.; Toma, H. E.; Anal. Chim. Acta 2002, 452, 23.
32. Araki, K.; Winnischofer, H.; Viana, H. E. B.; Toyama, M. M.; Engelmann, F. M.; Mayer, I.; Formiga, A. L. B.; Toma, H. E.; J. Electroanal. Chem. 2004, 562, 145.
33. Wu, F. H.; Zhao, G. C.; Wei, X. W.; Electrochem. Comm. 2002, 4, 690.
34. Rocha, J. R. C.; Angnes, L.; Bertotti, M.; Araki, K.; Toma, H. E.; Anal. Chim. Acta 2002, 452, 23.
35. Azevedo, C. M. N.; Araki, K.; Toma, H. E.; Angnes, L.; Anal. Chim. Acta 1999, 387, 175.
36. Li, X.; Fu, Y.; Sun, C.; Electroanalysis 2003, 15, 1707.
37. Mayer, I.; Formiga, A. L. B.; Engelmann, F. M.; Winnischofer, H.; Oliveira, P. V.; Tomazela, D. M.; Eberlin, M. N.; Toma, H. E.; Araki, K.; Inorg. Chim. Acta 2005, in press.
38. Toyama, M. M.; Demets, G. J. F.; Araki, K.; Toma, H. E.; Electrochem. Comm. 2000, 2, 749.
39. Engelmann, F. M.; Losco, P.; Winnischofer, H.; Araki, K.; Toma, H. E.; J. Porphyr. Phthalocyanines 2002, 6, 33.
40. Tomazela, D. M.; Gozzo, F. C.; Mayer, I.; Engelmann, F. M.; Araki, K.; Toma, H. E.; Eberlin, M. N.; J. Mass. Spectrom. 2004, 39, 1161.
41. Dovidauskas, S.; Araki, K.; Toma, H. E.; J. Porphyr. Phthalocyanines 2000, 4, 727.
42. Araki, K.; Toma, H. E.; J. Coord. Chem. 1993, 30, 9.
43. Vogel, G.C.; Beckmann, B. A.; Inorg. Chem. 1976, 15, 483.
44. Bhyrappa, P.; Krishnan, V.; Nethaji, M.; J. Chem. Soc. Dalton Trans. 1993, 12, 1901.
45. Araki, K.; Toma, H. E.; J. Photochem. Photobiol. A-Chem. 1994, 83, 245.
46. Araki, K.; Toma, H. E.; J. Chem. Res. S 1994, 7, 290.
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