期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 19, 期 29, 页码 9644-9654出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201203846
关键词
electrophilicity; intermolecular hardness; manganese porphyrins; metalloporphyrins; oxygen reduction
资金
- Germany Academic Exchange Service (DAAD)
- Helmholtz-Energie-Allianz Stationare elektrochemische Speicher und Wandler [HA-E-0002]
- Cluster of Excellence RESOLV [DFG EXC-1069]
Incisive modulation of the intermolecular hardness between metalloporphyrins and O-2 can lead to the identification of promising catalysts for oxygen reduction. The dependency of the electrocatalytic reduction of O-2 by metalloporphyrins on the nature of the central metal yields a volcano-type curve, which is rationalized to be in accordance with the Sabatier principle by using an approximation of the electrophilicity of the complexes. By using electrochemical and UV/Vis data, the influence of a selection of meso-substituents on the change in the energy for the * excitation of manganese porphyrins was evaluated allowing one to quantitatively correlate the influence of the various ligands on the electrocatalysis of O-2 reduction by the complexes. A manganese porphyrin was identified that electrocatalyzes the reduction of oxygen at low overpotentials without generating hydrogen peroxide. The activity of the complex became remarkably enhanced upon its pyrolysis at 650 degrees C.
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