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Potential-driven surface active structure rearrangement over FeP@NC towards efficient electrocatalytic hydrogen

Fumin Tang1, Hui Su, Xu Zhao

  • 1National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, Anhui, P. R. China. weiren@ustc.edu.cn.

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Summary

This study introduces FeP@NC, an efficient electrocatalyst for the hydrogen evolution reaction (HER). It demonstrates a dynamic structural change during HER, enhancing catalytic activity and stability.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Optimizing electrocatalysts for the hydrogen evolution reaction (HER) requires understanding active site structural dynamics.
  • Iron phosphide (FeP) based materials are promising for HER but require structural modification for enhanced performance.

Purpose of the Study:

  • To synthesize and characterize a novel FeP-based electrocatalyst with enhanced HER activity and stability.
  • To investigate the in situ structural evolution of the electrocatalyst during the HER process.

Main Methods:

  • Pyrolysis and equivalent-volume impregnation for FeP@NC composite synthesis.
  • In situ X-ray absorption spectroscopy (XAS) to probe structural changes.
  • Electrochemical measurements (overpotential, current density, stability).
  • Theoretical calculations to elucidate reaction mechanisms.

Main Results:

  • FeP@NC exhibits efficient HER with a low overpotential (135 mV at 10 mA cm⁻²) and robust stability (>15 h).
  • In situ XAS reveals a potential-dependent surface rearrangement from pentahedral to octahedral Fe structures via hydroxylation during HER.
  • Theoretical calculations confirm that the rearranged FeP₅(OH) structure facilitates proton acceptance at adjacent P sites, improving Volmer step kinetics.

Conclusions:

  • The dynamic structural rearrangement of FeP@NC under HER conditions is key to its high electrocatalytic performance.
  • The N-doped carbon coating and the in situ formed octahedral Fe moiety contribute to efficient proton adsorption and hydrogen evolution.
  • This work provides insights into designing advanced electrocatalysts by controlling active site structural evolution.