ISBN: 978-83-60043-10-3 - eurobic9

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Eurobic9, 2-6 September, 2008, Wrocław, Poland P89. Coordination Modes and Structural Aspects of Mixed-ligand Copper(II) Complexes Containing Some Polyamines and Amino Acids A. Kamecka a , K. Bogusz a , J. Jezierska . b , A. Woźna. a , B. Kurzak a a Department of Chemistry, University of Podlasie, 3 Maj 54, 08-110, Siedlce, Poland b Faculty of Chemistry, University of Wrocław, F. Joliot Curie 14, 50-383, Wrocław, Poland Amino acids and peptides, which are the basic structural units of proteins, are potential chelating reagents for copper(II) ion [1, 2]. There is continuing interest in coordination compounds of copper(II) with various combinations of heterocyclic nitrogen, thiolate and thioether donors because of the coordination of copper to two histidine nitrogen atoms and cysteine and methionine sulfur atoms in the electron transfer blue copper proteins [3, 4]. Furthermore, in a number of biochemical processes copper(II) is involved in mixed-ligand complex formation and ligand catalysed complex formation reactions [5]. Due to the fact that polyamines are found at a significant concentration in young cells and, particularly, in cancer tumor tissues [6], it seems to be interesting to investigate the ternary copper(II)-polyamine-histidine/methionine systems (the polyamines such as ethylenediamine (en), diethylenetriamine (dien) or N, N, N’, N’’, N’’-pentamethyldiethylenetriamine (Me5dien)). The stoichiometries, stability constants and bonding modes of the species formed at aqueous solution in the copper(II) ternary systems have been established. Our spectroscopic results indicate the tetragonal geometry for the mixed-ligand complexes of en, the geometry slightly deviated from square pyramidal for the species of dien and strongly deviated from square pyramidal towards trigonal bipyramidal for the complexes of Me5dien. References: [1] P. Deschamps, P.P. Kulkarni, M. Gautam-Basak, B. Sarkar, Coord. Chem. Rev., 249 (2005) 895. [2] B.G. Malstrom, J. Leckner, Current Opinion in Chemical Biology, 2 (1998) 286. [3] E.I. Solomon, M.J. Baldwin, M.D. Lowery, Chem. Rev. 92 (1992) 521. [4] E.I. Solomon, R.K. Szilagyi, S.D. Georgie, L. Basumallick, Chem. Rev. 104 (2004) 419. [5] H. Sigel, Metal Ions in Biological Systems, Vol.3, Marcel Dekker Inc., New York, 1974. [6] C.W. Tabor, H. Tabor, Ann. Rev. Biochem. 53 (1984) 749. _____________________________________________________________________ 208
Eurobic9, 2-6 September, 2008, Wrocław, Poland P90. Mechanism for Autoxidation of Nitric Oxide Adduct of Manganese(II) Porphyrin Placed in Microscopically Hydrophobic Environments in Aqueous Solution K. Kano, Y. Itoh, H. Kitagishi a Molecular Chemistry and Biochemistry, Doshisha University, Tatara, 610-0321, Kyotanabe, Japan e-mail:kkano@mail.doshisha.ac.jp Nitric oxide (NO) is bound to various hemoproteins to inhibit or activate protein functions. Since NO induces oxidation of oxyMb yielding inactive metMb, the mechanism for oxidation of oxyMb by NO has been well studied and established. Meanwhile, Mb binds NO and (NO)Mb is gradually oxidized to metMb and NO3 - . However, the mechanism for oxidation of (NO)Mb by dioxygen has not been clarified. Recently, we demonstrated the mechanism for oxidation of the NO adduct of a Mb model [1]. In this work, we studied the mechanism for oxidation of the NO adduct of 5,10,15,20-tetrakis(4-sulfonatophenyl)porphinato manganese(II) (Mn(II)TPPS) complexed with a model protein to confirm our previous mechanism. The model system is composed of a per-O-methylated beta-cyclodextrin dimer (Py2CD) having a pyridine linker and Mn(II)TPPS. Py2CD formed an extremely stable 1:1 inclusion complex (Mn(II)PCD) of Mn(II)TPPS in aqueous phosphate buffer solution at pH 7.0. Mn(II)PCD bound NO and (NO)Mn(II)PCD was gradually oxidized to Mn(III)PCD and NO3 - under aerobic conditions, the half-life time being ~35 h. The oxidation obeyed the zero-order kinetics, suggesting that NO gradually dissociates from its adduct (rate-determining step) and Mn(II)TPPS formed is autoxidized by dioxygen affording Mn(III)PCD and superoxide. The superoxide anion immediately reacts with NO to yield NO3 - . The present study supports the previous mechanism for (NO)Fe(II)PCD [1]. References: [1]K. Kano, Y. Itoh, H. Kitagishi, T. Hayashi, S. Hirota, J. Am. Chem. Soc., in press _____________________________________________________________________ 209
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ISBN: 978-83-60043-10-3 - eurobic9

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