Dinuclear Cu-2(II,II)-cores stabilized by the N3O donorset of HL1 = (2-{[[di(2-pyridyl)methyl](methyl)amino]methyl}phenol), HL2 = 2-({[di(2-pyridyl)methyl] amino}methyl)phenol), and HL3 = 2-({[di(2-pyridyl)methyl]amino}methyl)-4-nitrophenol display a unique superoxide dismutase (SOD) combined with catalase (CAT)-like activity in water, at neutral pH. The Cu2L21 < Cu2L22 < Cu2L23 structure-reactivity trend puts a spotlight on the electron-deficient core of Cu2L23 that exhibits the highest SOD (log k(cat) (O-2(center dot-)) = 7.55) and CAT-like (k(H2O2) = 0.66 M(-1)s(-1)) performance. Time-lapse ESI-MS and EPR experiments indicate that a dimeric core is essential for oxygenic turnover upon H2O2 decomposition.
Neutralization of Reactive Oxygen Species at Dinuclear Cu(II)-Cores: Tuning the Antioxidant Manifold in Water by Ligand Design
Neal Hickey;R. De Zorzi;Silvano Geremia;
2020-01-01
Abstract
Dinuclear Cu-2(II,II)-cores stabilized by the N3O donorset of HL1 = (2-{[[di(2-pyridyl)methyl](methyl)amino]methyl}phenol), HL2 = 2-({[di(2-pyridyl)methyl] amino}methyl)phenol), and HL3 = 2-({[di(2-pyridyl)methyl]amino}methyl)-4-nitrophenol display a unique superoxide dismutase (SOD) combined with catalase (CAT)-like activity in water, at neutral pH. The Cu2L21 < Cu2L22 < Cu2L23 structure-reactivity trend puts a spotlight on the electron-deficient core of Cu2L23 that exhibits the highest SOD (log k(cat) (O-2(center dot-)) = 7.55) and CAT-like (k(H2O2) = 0.66 M(-1)s(-1)) performance. Time-lapse ESI-MS and EPR experiments indicate that a dimeric core is essential for oxygenic turnover upon H2O2 decomposition.File | Dimensione | Formato | |
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