Rationalizing the Influence of the Mn(IV)/Mn(III) Red-Ox Transition on the Electrocatalytic Activity of Manganese Oxides in the Oxygen Reduction Reaction

被引：99

作者：

Ryabova, Anna S. ^{[1
,2
]}

Napolskiy, Filipp S. ^{[1
]}

Poux, Tiphaine ^{[2
]}

Istomin, Sergey Ya. ^{[1
]}

Bonnefont, Antoine ^{[3
]}

Antipin, Denis M. ^{[1
]}

Baranchikov, Alexander Ye. ^{[4
]}

Levin, Eduard E. ^{[1
]}

Abakumov, Artem M. ^{[5
]}

Kerangueven, Gwenaelle ^{[2
]}

Antipov, Evgeny V. ^{[1
]}

Tsirlina, Galina A. ^{[1
]}

Savinova, Elena R. ^{[2
]}

机构：

[1] Moscow MV Lomonosov State Univ, Moscow 119991, Russia

[2] Univ Strasbourg, ICPEES, UMR 7515, CNRS,ECPM, F-67087 Strasbourg 2, France

[3] Univ Strasbourg, CNRS, UMR 7177, IC, F-67000 Strasbourg, France

[4] Kurnakov Inst Gen & Inorgan Chem RAS, Moscow 119991, Russia

[5] Univ Antwerp, EMAT, Dept Phys, B-2020 Antwerp, Belgium

来源：

ELECTROCHIMICA ACTA | 2016年 / 187卷

基金：

俄罗斯基础研究基金会;

关键词：

Manganese oxides; Oxygen reduction reaction (ORR); Interfacial Red-ox transition; Rotating disc electrode (RDE); Meanfield kinetic modeling; CARBON; CATALYSTS; PEROVSKITE; ELECTRODE; NANOPARTICLES; DIFFRACTION; COMPOSITES; OXIDATION; BEHAVIOR; SUPPORT;

D O I：

10.1016/j.electacta.2015.11.012

中图分类号：

O646 [电化学、电解、磁化学];

学科分类号：

081704 ;

摘要：

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.

引用

页码：161 / 172

页数：12

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