Effect of the chemical order on the electrocatalytic activity of model PtCo electrodes in the oxygen reduction reaction

被引:43
作者
Lebedeva, Marina V. [1 ]
Pierron-Bohnes, Veronique [2 ]
Goyhenex, Christine [2 ]
Papaefthimiou, Vasiliki [1 ]
Zafeiratos, Spyridon [1 ]
Nazmutdinov, Renat R. [4 ]
Da Costa, Victor [2 ]
Acosta, Manuel [2 ]
Zosiak, Lukasz [2 ,3 ]
Kozubski, Rafal [3 ]
Muller, Dominique [5 ,6 ]
Savinova, Elena R. [1 ]
机构
[1] Univ Strasbourg, CNRS, ICPEES, UMR 7515, F-67087 Strasbourg, France
[2] Univ Strasbourg, CNRS, IPCMS, UMR 7504, F-67034 Strasbourg 2, France
[3] Jagiellonian Univ, M Smoluchowski Inst Phys, PL-30059 Krakow, Poland
[4] Kazan Natl Res Technol Univ, Kazan 420015, Russia
[5] Univ Strasbourg, ICube, F-67037 Strasbourg 2, France
[6] CNRS, F-67037 Strasbourg 2, France
关键词
Electrocatalysis; Oxygen reduction reaction; Ordered PtCo alloys; Density functional theory; Adiabatic electron transfer; Spin effects; MAGNETIC-PROPERTIES; STEPPED SURFACES; CO ALLOYS; STABILITY; CATALYSTS; KINETICS; POTENTIALS; TRANSITION; MONOLAYER; DENSITY;
D O I
10.1016/j.electacta.2013.07.038
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
PtCo alloys have long been known to possess higher activity in the electrochemical oxygen reduction reaction compared to pure Pt. This work addresses the influence of the chemical order on the electrocatalytic activity of PtCo alloy, the phenomenon, which has been already documented in the literature but yet poorly understood. Single crystalline PtCo(0 01) alloy films were epitaxially grown on Mg(0 0 1) substrates and used as model electrodes to study the influence of the chemical order on the electrochemical oxygen reduction reaction. Electrodes with close Pt:Co atomic ratios in the bulk and near surface region show grossly different electrocatalytic activities against the chemical order, the ordered L1(0) phase being ca. 7 times more active than the disordered fcc A1 structure. Electronic structure calculations and quantum mechanical theory of electron transfer are utilized to provide a rational for this remarkable phenomenon. (C) 2013 Elsevier Ltd. All rights reserved.
引用
收藏
页码:605 / 616
页数:12
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