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Operando X-ray spectroscopic tracking of self-reconstruction for anchored nanoparticles as high-performance electrocatalysts towards oxygen evolution†
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2018-07-06 00:00:00 , DOI: 10.1039/c8ee00773j
Sanzhao Song 1, 2, 3, 4, 5 , Jing Zhou 1, 2, 3, 4 , Xiaozhi Su 1, 2, 3, 4 , Yu Wang 1, 2, 3, 4 , Jiong Li 1, 2, 3, 4 , Linjuan Zhang 1, 2, 3, 4 , Guoping Xiao 1, 2, 3, 4 , Chengzhi Guan 1, 2, 3, 4 , Renduo Liu 1, 2, 3, 4 , Shuguang Chen 1, 2, 3, 4 , Hong-Ji Lin 4, 6, 7 , Shuo Zhang 1, 2, 3, 4 , Jian-Qiang Wang 1, 2, 3, 4, 5
Affiliation  

Exploring high-performance electrocatalysts for the oxygen evolution reaction (OER) is pivotal for renewable energy storage and conversion. The surface self-reconstruction during the OER is considered as the key of highly active catalysts, whereas identifying the local electronic and geometric structure of the reconstruction-derived components is challenging. Herein, an in situ exsolution method towards the typical LaCo0.8Fe0.2O3−δ perovskite is developed to obtain a new type of lanthana-anchored CoFe catalyst. The optimized catalyst exhibits a low overpotential of 293 mV to reach the current density of 10 mA cm−2 in 0.1 M KOH. Most importantly, operando X-ray absorption spectroscopy (XAS) measurements demonstrate that the CoFe species in the catalyst are nearly transformed into unique (Co/Fe)O(OH) with a definite coordination-unsaturated structure under electrochemical conditions, which actually contributes to this superior performance. Moreover, the presence of the lanthana support promotes this transformation. Our work not only suggests a facile reconstructive strategy to dramatically enhance the OER activity of perovskite oxides in alkaline media, but also unravels the fine structure of true active sites through operando X-ray spectroscopic tracking.

中文翻译:

Operando X射线光谱对锚定纳米颗粒的自我重建的追踪,作为对氧气逸出的高性能电催化剂

探索用于氧气释放反应(OER)的高性能电催化剂对于可再生能源的存储和转化至关重要。OER过程中的表面自我重建被认为是高活性催化剂的关键,而如何识别源自重建的组分的局部电子和几何结构却具有挑战性。在本文中,在原位朝向典型LACO出溶方法0.80.2 ø 3- δ的钙钛矿被显影以获得新型氧化镧-锚定的CoFe催化剂。优化的催化剂表现出293 mV的低过电势,以在0.1 M KOH中达到10 mA cm -2的电流密度。最重要的是,操作X射线吸收光谱(XAS)测量表明,在电化学条件下,催化剂中的CoFe物质几乎转化为具有确定的配位不饱和结构的独特(Co / Fe)O(OH),实际上有助于实现这一优异性能。此外,lanthana支持的存在促进了这种转变。我们的工作不仅意味着一个浅显的重建策略,极大地提高在碱性介质中钙钛矿氧化物的OER活动,同时也揭开了通过真正的活性位点的精细结构operando X射线光谱跟踪。
更新日期:2018-07-06
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