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Operando X-ray Spectroscopic Tracking of Self-reconstruction for Anchored Nanoparticles as High-performance Electrocatalysts Towards Oxygen Evolution
S. Song, J. Zhou, X. Su, Y. Wang*, J. Li, L. Zhang, G. Xiao, C. Guan, R. Liu, S. Chen, H.-J. Lin, S. Zhang*, and J.-Q. Wang*
2018/12/03
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.