Highly Active and Stable Iridium Pyrochlores for Oxygen Evolution Reaction

被引:205
作者
Lebedev, Dmitry [1 ]
Povia, Mauro [2 ]
Waltar, Kay [2 ,7 ]
Abdala, Paula M. [3 ]
Castelli, Ivano E. [4 ,5 ]
Fabbri, Emiliana [2 ]
Blanco, Maria V. [6 ]
Fedorov, Alexey [1 ,3 ]
Coperet, Christophe [1 ]
Marzari, Nicola [4 ,5 ]
Schmidt, Thomas J. [1 ,2 ]
机构
[1] ETH, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1-5, CH-8093 Zurich, Switzerland
[2] Paul Scherrer Inst, Electrochem Lab, CH-5232 Villigen, Switzerland
[3] ETH, Dept Mech & Proc Engn, Leonhardstr 21, CH-8092 Zurich, Switzerland
[4] Ecole Polytech Fed Lausanne, Theory & Simulat Mat THEOS, CH-1015 Lausanne, Switzerland
[5] Ecole Polytech Fed Lausanne, Natl Ctr Computat Design & Discovery Novel Mat MA, CH-1015 Lausanne, Switzerland
[6] European Synchrotron Radiat Facil, BP 220, F-38043 Grenoble, France
[7] Univ Zurich, Dept Phys, Surface Phys Lab, Winterthurerstr 190, CH-8057 Zurich, Switzerland
基金
瑞士国家科学基金会;
关键词
HIGH-SURFACE-AREA; WATER OXIDATION; OXIDE; CATALYST; ELECTROCATALYSTS; ELECTROLYSIS; EFFICIENT; PEROVSKITES; ELECTRODES; STABILITY;
D O I
10.1021/acs.chemmater.7b00766
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Proton exchange membrane water electrolysis (PEMWE) is a promising technology for electricity-to-fuel conversion which allows for direct production of hydrogen from water. One of the key problems limiting widespread implementation of PEMWE into energy systems is the sluggish kinetics of the anodic process: the oxygen evolution reaction (OER). Additionally, state-of-the-art OER materials contain large amounts of low abundant noble metals (Ru, Ir), and therefore, development of low-cost, highly active and stable OER catalysts remains an important challenge. We developed a synthetic approach to the iridium pyrochlores complex oxides of iridium with reduced content of the noble metal as compared to IrO2. The materials were synthesized from molten sodium nitrate (Adams fusion method) at moderate temperatures (500-575 degrees C) and consist of highly crystalline iridium pyrochlore nanoparticles with surface areas of up to 40 m(2) C-1, which is a significant improvement compared to the traditional high temperature solid-state synthesis. Electrochemical measurements in acidic media showed that yttrium and bismuth pyrochlore catalysts possess high OER activity approaching the activity of state-of-the-art IrO2 nanoparticles. High intrinsic activities and stability behavior of yttrium iridium catalysts were correlated with the formation of the highly active IrOx surface layer due to leaching of the Y3+ cations into the electrolyte solution, revealed both experimentally and computationally using density functional theory calculations.
引用
收藏
页码:5182 / 5191
页数:10
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