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Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment
In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution
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Paper Summary
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NiFe and CoFe LDHs Get Squeezed for Oxygen! (Like a Sponge, But for Electrocatalysis)
This study reveals that NiFe and CoFe layered double hydroxides (LDHs) undergo a phase transition from the as-prepared α-phase to an active γ-phase under oxygen evolution reaction (OER) conditions, characterized by lattice compression. The OER proceeds via a Mars van Krevelen mechanism, with a synergistic O-bridged Fe-M reaction center (M = Ni or Co) stabilizing key intermediates and facilitating the high catalytic activity observed.
Possible Conflicts of Interest
None identified
Identified Weaknesses
Limited surface analysis
The study primarily focuses on the (01-10) surface for mechanistic analysis, neglecting other possible exposed surfaces at the edges of catalyst sheets. This limits the generalizability of the findings to the overall catalytic behavior.
Discrepancy between calculated and experimental overpotentials
While the overpotentials calculated using DFT are semi-quantitatively consistent with experimental measurements, there's still a noticeable difference. This gap suggests potential inaccuracies in the theoretical model or limitations in capturing the complex experimental conditions.
Incomplete phase transitions affecting XAS interpretation
The incomplete phase transition observed in the experiments complicates the interpretation of XAS data, as the measured properties become averaged across different phases. This makes it challenging to isolate the specific characteristics of the active y-phase.
Rating Explanation
This study presents a comprehensive investigation combining operando experiments, DFT calculations, and mechanistic studies to unravel the OER mechanism on NiFe and CoFe LDHs. The identification of the active y-phase and the elucidation of the synergistic reaction center represent significant contributions to the field. While limitations exist regarding surface analysis, the quantitative agreement between theoretical and experimental results, and the incomplete phase transition, the overall methodology and findings are robust, warranting a rating of 4.
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Original Title:
In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution
File Name:
s41467-020-16237-1.pdf
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File Size:
1.86 MB
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July 14, 2025 at 10:35 AM
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