4.8 Article

Surface Fluorination Engineering of NiFe Prussian Blue Analogue Derivatives for Highly Efficient Oxygen Evolution Reaction

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 4, Pages 5142-5152

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c20886

Keywords

oxygen evolution reaction; NiFe-PBAs-F; fluorination engineering; dramatic reconstruction; lattice oxygen oxidation mechanism

Funding

  1. Natural Science Foundation of Shandong Province [ZR2019QB005]
  2. National Natural Science Foundation of China [22072072, 21802087, 51972195, 21832005, 21972078]
  3. National Key Research and Development Program of China [2020YFA0710301]
  4. Shandong University multidisciplinary research and innovation team of young scholars [2020QNQT11, 2020QNQT012]
  5. Shandong University
  6. Taishan Scholar Foundation of Shandong Province

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Surface engineering plays a crucial role in enhancing the electrocatalytic performance of NiFe-PBA-F catalyst for oxygen evolution reaction (OER). The controlled removal of ligands through surface fluorination provides a pathway for maintaining the framework structure of NiFe-PBA, leading to the creation of more active sites for F-doped NiFeOOH. The lattice oxygen oxidation mechanism proposed for NiFe-PBA-F contributes to a better understanding of the reconstruction process and the OER mechanism.
Surface engineering is of importance to reduce the reaction barrier of oxygen evolution reaction (OER). Herein, the NiFe Prussian blue analogue (NiFe-PBA)-F catalyst with a multilevel structure was obtained from NiFe-PBAs via a fluorination strategy, which presents an ultralow OER overpotential of 190 mV at 10 mA cm(-2) in alkaline solution, with a small Tafel slope of 57 mV dec(-1) and excellent stability. Interestingly, surface fluorination engineering could achieve a controllable removal of ligands of the cyan group, contributing to keep the framework structure of NiFe-PBAs. Particularly, NiFe-PBAs-F undergoes a dramatic reconstruction with the dynamic migration of F ions, which creates more active sites of F-doped NiFeOOH and affords more favorable adsorption of oxygen intermediates. Density functional theory calculations suggest that F doping increases the state density of Ni 3d orbital around the Fermi level, thus improving the conductivity of NiFeOOH. Furthermore, based on our experimental results, the lattice oxygen oxidation mechanism for NiFe-PBAs-F was proposed. Our work not only provides a new pathway to realize the controllable pyrolysis of NiFe-PBAs but also gives more insights into the reconstruction and the mechanism for the OER process.

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