Highly Active and Stable Iridium Pyrochlores for Oxygen Evolution Reaction

作者:Lebedev Dmitry; Povia Mauro; Waltar Kay; Abdala Paula M; Castelli Ivano E; Fabbri Emiliana; Blanco Maria V; Fedorov Alexey; Coperet Christophe; Marzari Nicola*; Schmidt Thomas J*
来源:Chemistry of Materials, 2017, 29(12): 5182-5191.
DOI:10.1021/acs.chemmater.7b00766

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.

  • 出版日期2017-6-27