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In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution
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In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution
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Journal Article
In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution
2020
Overview
NiFe and CoFe (MFe) layered double hydroxides (LDHs) are among the most active electrocatalysts for the alkaline oxygen evolution reaction (OER). Herein, we combine electrochemical measurements,
operando
X-ray scattering and absorption spectroscopy, and density functional theory (DFT) calculations to elucidate the catalytically active phase, reaction center and the OER mechanism. We provide the first direct atomic-scale evidence that, under applied anodic potentials, MFe LDHs oxidize from as-prepared α-phases to activated γ-phases. The OER-active γ-phases are characterized by about 8% contraction of the lattice spacing and switching of the intercalated ions. DFT calculations reveal that the OER proceeds via a Mars van Krevelen mechanism. The flexible electronic structure of the surface Fe sites, and their synergy with nearest-neighbor M sites through formation of O-bridged Fe-M reaction centers, stabilize OER intermediates that are unfavorable on pure M-M centers and single Fe sites, fundamentally accounting for the high catalytic activity of MFe LDHs.
NiFe and CoFe layered double hydroxides are among the most active electrocatalysts for the alkaline oxygen evolution reaction. Here, by combining
operando
experiments and rigorous DFT calculations, the authors unravel their active phase, the reaction center and the catalytic mechanism.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
