Mechanistic insight on the catecholase activity of dinuclear copper complexes with distant metal centers


Por: Mendoza-Quijano M.R., Ferrer-Sueta G., Flores-Álamo M., Aliaga-Alcalde N., Gómez-Vidales V., Ugalde-Saldívar V.M., Gasque L.

Publicada: 1 ene 2012
Categoría: Inorganic Chemistry

Resumen:
The catecholase activity of two dinuclear Cu(II) complexes with distant metal centers is discussed together with solid state and solution studies. The crystal structure for one of them, [Cu-2(diep)(H2O)(4)] (ClO4)(4)center dot 2H(2)O, is described, showing the two copper ions are 7.457 angstrom apart and in a square pyramidal coordination. Both complexes display a weak antiferromagnetic coupling in the solid state that is manifest in the dimer EPR spectra obtained in frozen solution. The pH-potentiometric speciation performed in 1 : 1 MeOH H2O allowed the assignment of hydrolyzed copper species as those catalytically active in the oxidation of 3,5-di-tert-butylcatechol (DTBC). The kinetic measurements led us to propose behavior consistent with Michaelis-Menten plus a linear dependence of the initial rate on [DTBC]. This can be associated with the presence of more than one catalytically active species, which is consistent with the evidence of several differently hydrolyzed species shown

Filiaciones:
Mendoza-Quijano M.R.:
 Univ Nacl Autonoma Mexico, Dept Quim Inorgan & Nucl, Fac Quim, Mexico City 04510, DF, Mexico

Ferrer-Sueta G.:
 Laboratorio de Fisicoquímica Biológica, Facultad de Ciencias, Universidad de la República Iguá, 4225 11400 Montevideo, Uruguay

Flores-Álamo M.:
 Univ Nacl Autonoma Mexico, Dept Quim Inorgan & Nucl, Fac Quim, Mexico City 04510, DF, Mexico

Aliaga-Alcalde N.:
 ICREA-Departament de Química Inorgànica, Universitat de Barcelona Diagonal, 645 08028 Barcelona, Spain

Gómez-Vidales V.:
 Univ Nacl Autonoma Mexico, Inst Quim, Mexico City 04510, DF, Mexico

Ugalde-Saldívar V.M.:
 Univ Nacl Autonoma Mexico, Dept Quim Inorgan & Nucl, Fac Quim, Mexico City 04510, DF, Mexico

Gasque L.:
 Univ Nacl Autonoma Mexico, Dept Quim Inorgan & Nucl, Fac Quim, Mexico City 04510, DF, Mexico
ISSN: 14779226
Editorial
ROYAL SOC CHEMISTRY, THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND, Reino Unido
Tipo de documento: Article
Volumen: 41 Número: 16
Páginas: 4985-4997
WOS Id: 000302023800036
ID de PubMed: 22411076