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Operando unveiling the activity origin via preferential structural evolution in Ni-Fe (oxy)phosphides for efficient

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Non-noble metal catalysts show promise for the oxygen evolution reaction (OER). This study reveals that an in situ generated O-Fe-P structure in Ni-Fe phosphides is the key to their enhanced OER activity.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Non-noble metal-based heteroatom compounds exhibit significant electrocatalytic activity for the oxygen evolution reaction (OER).
  • Understanding the structure-activity relationship is crucial for optimizing these catalysts, but is hindered by a lack of effective in situ/operando characterization techniques.
  • Ni-Fe bimetallic phosphides are promising OER electrocatalysts, yet their reaction mechanism and active site origins require further elucidation.

Purpose of the Study:

  • To establish a direct structure-activity correlation for OER catalysts using advanced operando techniques.
  • To elucidate the origin of the enhanced electrocatalytic activity in Ni-Fe bimetallic phosphides.
  • To provide insights for the rational design of next-generation OER electrocatalysts.

Main Methods:

  • Operando quick-scan X-ray absorption fine structure (Q-XAFS) spectroscopy.
  • In situ electrochemical potential control.
  • Theoretical calculations (e.g., DFT).

Main Results:

  • Operando Q-XAFS revealed that structural transformation begins with the preferential oxidation of Fe sites over Ni sites.
  • The in situ formation of an O-Fe-P structure was identified as the origin of the enhanced OER activity.
  • Theoretical calculations corroborated the experimental findings, confirming the role of the O-Fe-P structure.

Conclusions:

  • The study successfully correlated catalyst structure evolution with OER activity using operando Q-XAFS.
  • The preferential oxidation of Fe and the subsequent formation of the O-Fe-P structure are critical for high OER performance in Ni-Fe phosphides.
  • These findings advance the mechanistic understanding of Ni-Fe-based OER electrocatalysts and guide future catalyst design.