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表面氧空位和钌价态对烧绿石氧化物催化性能的影响

Influence of Surface Oxygen Vacancies and Ruthenium Valence State on the Catalysis of Pyrochlore Oxides.

作者信息

Feng Qi, Zou Jiexin, Wang Yajun, Zhao Zhiliang, Williams Mark C, Li Hui, Wang Haijiang

机构信息

School of Materials Science and Engineering , Harbin Institute of Technology , Harbin 150001 , China.

Department of Materials Science and Engineering, Shenzhen Key Laboratory of Hydrogen Energy , Southern University of Science and Technology , Shenzhen 518055 , Guangdong , China.

出版信息

ACS Appl Mater Interfaces. 2020 Jan 29;12(4):4520-4530. doi: 10.1021/acsami.9b19352. Epub 2020 Jan 13.

Abstract

Proton exchange membrane (PEM) water electrolysis is a promising energy storage solution by electrochemically splitting water into hydrogen fuel and oxygen. However, the sluggish kinetics, high operating potential, and corrosive acidic environment during the oxygen evolution reaction (OER) require the use of scarce and costly Ir-based oxides, tremendously hampering its large-scale commercialization. Hence, developing active and stable anode catalysts with reduced precious-metal usage is desperately essential. For the first time, we report a group of YBaRuO pyrochlore oxides and employ them in acid OER and PEM electrolyzers. We reveal the mechanism for the promoted OER performance of Ba-doped YRuO in which partially replacing Y by Ba in YRuO greatly facilitates the hole-doping effect, which generates massive oxygen vacancy and multivalence of Ru/Ru, thus boosting the OER performance of YBaRuO. This work provides an effective method and paradigm for improving the electrocatalytic property of pyrochlore oxides.

摘要

质子交换膜(PEM)水电解是一种很有前景的储能解决方案,它通过将水电化学分解为氢燃料和氧气来实现。然而,析氧反应(OER)过程中缓慢的动力学、高工作电位以及腐蚀性的酸性环境需要使用稀缺且昂贵的铱基氧化物,这极大地阻碍了其大规模商业化。因此,开发活性高且稳定的阳极催化剂并减少贵金属的使用极为关键。我们首次报道了一组钇钡钌氧(YBaRuO)烧绿石氧化物,并将其应用于酸性OER和PEM电解槽中。我们揭示了钡掺杂YRuO促进OER性能的机制,即在YRuO中用Ba部分替代Y极大地促进了空穴掺杂效应,这产生了大量的氧空位以及Ru/Ru的多价态,从而提高了YBaRuO的OER性能。这项工作为改善烧绿石氧化物的电催化性能提供了一种有效的方法和范例。

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