Operando X-ray spectroscopic tracking of self-reconstruction for anchored nanoparticles as high-performance electrocatalysts towards oxygen evolution
Operando X-ray spectroscopic tracking of self-reconstruction for anchored nanoparticles as high-performance electrocatalysts towards oxygen evolution
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锚定纳米颗粒作为高性能析氧电催化剂的自重建操作 X 射线光谱跟踪
DOI：
10.1039/c8ee00773j
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发表时间：
2018-10
影响因子：
32.5
通讯作者：
Wang Jian-Qiang
中科院分区：
文献类型：
--
作者：
Song Sanzhao;Zhou Jing;Su Xiaozhi;Wang Yu;Li Jiong;Zhang Linjuan;Xiao Guoping;Guan Chengzhi;Liu Renduo;Chen Shuguang;Lin Hong-Ji;Zhang Shuo;Wang Jian-Qiang
开发用于析氧反应（OER）的高性能电催化剂是可再生能源储存和转换的关键。OER过程中的表面自重构被认为是高活性催化剂的关键，而识别重构衍生组分的局部电子和几何结构具有挑战性。在此，开发了一种针对典型的LaCo0.8Fe0.2O3−δ钙钛矿的原位出溶方法，以获得新型的氧化镧锚定的CoFe催化剂。优化的催化剂表现出293 mV的低过电位，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）的测量表明，在催化剂中的CoFe物种几乎转化为独特的（Co/Fe）O（OH）具有一定的配位不饱和结构的电化学条件下，这实际上有助于这种上级性能。此外，氧化镧载体的存在促进了这种转化。我们的工作不仅提出了一种简单的重建策略，以显着提高钙钛矿氧化物在碱性介质中的OER活性，而且还通过操作X射线光谱跟踪揭示了真正的活性位点的精细结构。
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.
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