期刊
ELECTROCHIMICA ACTA
卷 187, 期 -, 页码 161-172出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2015.11.012
关键词
Manganese oxides; Oxygen reduction reaction (ORR); Interfacial Red-ox transition; Rotating disc electrode (RDE); Meanfield kinetic modeling
资金
- CNRS (France)
- Russian Foundation for Basic Research [13-03-91054]
- French Ministry of Foreign Affairs and International Development for Eiffel scholarship
Knowledge on the mechanisms of oxygen reduction reaction (ORR) and descriptors linking the catalytic activity to the structural and electronic properties of transition metal oxides enable rational design of more efficient catalysts. In this work ORR electrocatalysis was studied on a set of single and complex Mn (III) oxides with a rotating disc electrode method and cyclic voltammetry. We discovered an exponential increase of the specific electrocatalytic activity with the potential of the surface Mn(IV)/Mn(III) red-ox couple, suggesting the latter as a new descriptor for the ORR electrocatalysis. The observed dependence is rationalized using a simple mean-field kinetic model considering availability of the Mn( III) centers and adsorbate-adsorbate interactions. We demonstrate an unprecedented activity of Mn2O3, ca. 40 times exceeding that of MnOOH and correlate the catalytic activity of Mn oxides to their crystal structure. (C) 2015 Elsevier Ltd. All rights reserved.
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