期刊
ELECTROCHIMICA ACTA
卷 191, 期 -, 页码 452-461出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2016.01.070
关键词
Electrocatalysis; Oxygen reduction; MnO2; DFT; Rational design
资金
- Danish Council for Strategic Research via the NACORR project [12-132695]
- European Commission in the framework of the Marie Curie Initial Training Network ELCAT [214936]
The paper focuses on theoretical and experimental aspects of an oxide surface optimization for oxygen reduction reaction (ORR). Various doped alpha-MnO2 based electrocatalysts were prepared by microwave-assisted hydrothermal synthesis and electrochemically characterized to validate density functional theory (DFT) based predictions of the oxidation state and local structure effects on the catalytic activity of alpha-MnO2 catalysts in ORR. Both theory and experiments conclude that the highest activity in ORR is to be expected in the case of clustered Mn3+ sites which yield activity comparable with that of the polycrystalline Pt. These active sites have to be formed under in-operando conditions and their formation is hindered in doped alpha-MnO2 catalysts. The activity of the other conceivable active sites based on non-clustered Mn3+ or Mn4+ is inferior to that of clustered Mn3+. The activation of Mn3+ or Mn4+ based active sites leads to a shift in selectivity of the ORR process towards 2 electron formation of hydrogen peroxide. (C) 2016 Elsevier Ltd. All rights reserved.
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