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Six Mn-Schiff base complexes, [Mn(X-salpn)]0/+ (salpn = 1,3-bis(sal-ic-ylidenamino)propane, X = H [1], 5-Cl [2], 2,5-F2 [3], 3,5-Cl2 [4], 5-NO2 [5], 3,5-(NO2)2 [6]), were synthesized and characterized in solution, and second-sphere effects on their electrochemical and spectroscopic properties were analyzed. The six complexes catalyze the dismutation of superoxide with catalytic rate constants in the range 0.65 to 1.54 × 106 M-1 s-1 obtained through the nitro blue tetrazolium photoreduction inhibition superoxide dismutases assay, in aqueous medium of pH 7.8. In solution, these compounds possess two labile solvent molecules in the axial positions favoring coordination of the highly nucleophilic O2 •- to the metal center. Even complex 5, [Mn(5-(NO2)salpn) (OAc) (H2O)], with an axial acetate in the solid state, behaves as a 1:1 electrolyte in methanolic solution. Electron paramagnetic resonance and UV-vis monitoring of the reaction of [Mn(X-salpn)]0/+ with KO2 demonstrates that in diluted solutions these complexes behave as catalysts supporting several additions of excess O2 •-, but at high complex concentrations (≥0.75 mM) catalyst self-inhibition occurs by the formation of a catalytically inactive dimer. The correlation of spectroscopic, electrochemical, and kinetics data suggest that second-sphere effects control the oxidation states of Mn involved in the O2 •- dismutation cycle catalyzed by complexes 1-6 and modulate the strength of the Mn-substrate adduct for electron-transfer through an inner-sphere mechanism. © 2019 American Chemical Society.


Documento: Artículo
Título:Insights into Second-Sphere Effects on Redox Potentials, Spectroscopic Properties, and Superoxide Dismutase Activity of Manganese Complexes with Schiff-Base Ligands
Autor:Palopoli, C.; Ferreyra, J.; Conte-Daban, A.; Richezzi, M.; Foi, A.; Doctorovich, F.; Anxolabéhère-Mallart, E.; Hureau, C.; Signorella, S.R.
Filiación:IQUIR (Instituto de Química Rosario), Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET), Facultad de Ciencias Bioquímicas y Farmacéuticas, Universidad Nacional de Rosario, Suipacha 531, Rosario, S2002LRK, Argentina
LCC-CNRS, Université de Toulouse, 205 route de Narbonne, Toulouse, 31077, France
Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE-CONICET, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria, Pabellón 2, Buenos Aires, C1428EHA, Argentina
Laboratoire d'Electrochimie Moléculaire UMR CNRS-P7 7591, Université Paris Diderot-Paris, 15 rue Jean-Antoine de Baïf, Paris Cedex 13, 75205, France
Página de inicio:48
Página de fin:57
Título revista:ACS Omega
Título revista abreviado:ACS Omega


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---------- APA ----------
Palopoli, C., Ferreyra, J., Conte-Daban, A., Richezzi, M., Foi, A., Doctorovich, F., Anxolabéhère-Mallart, E.,..., Signorella, S.R. (2019) . Insights into Second-Sphere Effects on Redox Potentials, Spectroscopic Properties, and Superoxide Dismutase Activity of Manganese Complexes with Schiff-Base Ligands. ACS Omega, 4(1), 48-57.
---------- CHICAGO ----------
Palopoli, C., Ferreyra, J., Conte-Daban, A., Richezzi, M., Foi, A., Doctorovich, F., et al. "Insights into Second-Sphere Effects on Redox Potentials, Spectroscopic Properties, and Superoxide Dismutase Activity of Manganese Complexes with Schiff-Base Ligands" . ACS Omega 4, no. 1 (2019) : 48-57.
---------- MLA ----------
Palopoli, C., Ferreyra, J., Conte-Daban, A., Richezzi, M., Foi, A., Doctorovich, F., et al. "Insights into Second-Sphere Effects on Redox Potentials, Spectroscopic Properties, and Superoxide Dismutase Activity of Manganese Complexes with Schiff-Base Ligands" . ACS Omega, vol. 4, no. 1, 2019, pp. 48-57.
---------- VANCOUVER ----------
Palopoli, C., Ferreyra, J., Conte-Daban, A., Richezzi, M., Foi, A., Doctorovich, F., et al. Insights into Second-Sphere Effects on Redox Potentials, Spectroscopic Properties, and Superoxide Dismutase Activity of Manganese Complexes with Schiff-Base Ligands. ACS Omega. 2019;4(1):48-57.