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Herein, we prepared a bimetallic layered double hydroxide (FeCo LDH) featuring a dandelion-like structure. Anchoring of CeO2 onto FeCo LDH produced interfaces between the functionalizing CeO2 and the parent LDH. Comparative electrochemical studies were carried out. Onset potential, overpotential, and Tafel slope point to the superior oxygen-evolving performance of CeO2-FeCo LDH with respect to FeCo LDH, therefore, demonstrating the merits of CeO2 functionalization. The electronic structures of Fe, Co, and Ce were analyzed by X-ray photoelectron spectroscopy (XPS) and electron energy loss spectroscopy (EELS) from which the increase of Co3+ and the concurrent lowering of Ce4+ were established. With the use of CeO2-FeCo LDH, accelerated formation at a sizably reduced potential of Co-OOH, one of the key intermediates preceding the release of O2was observed by in situ Raman spectroscopy. We now have the atomic-level and location-specific evidence, the increase of the active Co3+ across the interface to correlate the enhanced catalytic performance with CeO2 functionalization.
This work was financially supported by Shenzhen Nobel Prize Scientists Laboratory Project (No. C17213101), Guangdong Provincial Key Laboratory of Catalysis (No. 2020B121201002), Guangdong Provincial Key Laboratory of Energy Materials for Electric Power (No. 2018B030322001), China Postdoctoral Science Foundation (No. 2018M642133, X. Y. Z.), Post-doctorate Scientific Research Fund for staying (coming to) Shenzhen (No. K21217502, X. Y. Z.), the National Natural Science Foundation of China (No. 21671096, Z. G. L.) and Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials (No. ZDSYS20200421111401738, Z. G. L.). The authors also acknowledge the assistance of Southern University of Science and Technology Core Research Facilities (SUSTech CRF) and Key Laboratory of Energy Conversion and Storage Technologies (Southern University of Science and Technology).