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高性能焦绿石型钇钌酸电催化剂在酸性介质中用于氧析出反应。

High-Performance Pyrochlore-Type Yttrium Ruthenate Electrocatalyst for Oxygen Evolution Reaction in Acidic Media.

机构信息

Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign , 600 South Mathews Avenue, Urbana, Illinois 61801, United States.

X-ray Science Division, Argonne National Laboratory , 9700 South Cass Avenue, Argonne, Illinois 60439, United States.

出版信息

J Am Chem Soc. 2017 Aug 30;139(34):12076-12083. doi: 10.1021/jacs.7b06808. Epub 2017 Aug 17.

Abstract

Development of acid-stable electrocatalysts with low overpotential for oxygen evolution reaction (OER) is a major challenge to produce hydrogen directly from water. We report in this paper a pyrochlore yttrium ruthenate (YRuO) electrocatalyst that has significantly enhanced performance toward OER in acid media over the best-known catalysts, with an onset overpotential of 190 mV and high stability in 0.1 M perchloric acid solution. X-ray absorption near-edge structure (XANES) indicates YRuO electrocatalyst had a low valence state that favors the high OER activity. Density functional theory (DFT) calculation shows this pyrochlore has lower band center energy for the overlap between Ru 4d and O 2p orbitals and is therefore more stable Ru-O bond than RuO, highlighting the effect of yttrium on the enhancement in stability. The YRuO pyrochlore is also free of expensive iridium metal and thus is a cost-effective candidate for practical applications.

摘要

开发具有低过电位的酸稳定析氧反应 (OER) 电催化剂是直接从水中生产氢气的主要挑战。本文报道了一种钙钛矿钇钌酸盐 (YRuO) 电催化剂,在酸性介质中具有比最知名的催化剂显著增强的 OER 性能,其起始过电位为 190 mV,在 0.1 M 高氯酸溶液中具有高稳定性。X 射线吸收近边结构 (XANES) 表明 YRuO 电催化剂具有有利于高 OER 活性的低价态。密度泛函理论 (DFT) 计算表明,这种钙钛矿具有 Ru 4d 和 O 2p 轨道重叠的更低能带中心能量,因此比 RuO 具有更稳定的 Ru-O 键,突出了钇对稳定性增强的影响。YRuO 钙钛矿也不含昂贵的铱金属,因此是一种具有成本效益的实用应用候选材料。

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