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CoP for hydrogen evolution: implications from hydrogen adsorption.

Guoxiang Hu1, Qing Tang, De-En Jiang

  • 1Department of Chemistry, University of California, Riverside, CA 92521, USA. de-en.jiang@ucr.edu.

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Summary
This summary is machine-generated.

Cobalt phosphide (CoP) shows promise for hydrogen evolution reaction (HER) catalysis. DFT calculations reveal that CoP surfaces, particularly (111), exhibit favorable hydrogen adsorption, indicating excellent HER activity.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Computational Chemistry

Background:

  • Cobalt phosphide (CoP) is a highly promising earth-abundant electrocatalyst for the hydrogen evolution reaction (HER).
  • The precise mechanism governing CoP's catalytic activity, particularly hydrogen adsorption, remains incompletely understood.
  • Understanding hydrogen adsorption is crucial for optimizing HER electrocatalysts.

Purpose of the Study:

  • To investigate the adsorption of atomic hydrogen on various low-Miller-index surfaces of cobalt phosphide (CoP).
  • To elucidate the relationship between surface structure, hydrogen adsorption energetics, and HER activity.
  • To provide mechanistic insights into the high performance of CoP in HER.

Main Methods:

  • Periodic density functional theory (DFT) calculations were employed to study hydrogen adsorption.
  • Ab initio atomistic thermodynamics was used to determine surface stabilities under relevant conditions.
  • Gibbs free energy of adsorption was calculated to predict catalytic activity.

Main Results:

  • The (111), (110), and (011) CoP surfaces were predicted to exhibit good catalytic activity for HER.
  • Surface stability at 1 atm H2 and 300 K followed the trend: (111) > (100) ∼ (110) ≫ (011).
  • On the most stable (111) surface, hydrogen adsorption on Co bridge and P top sites showed near-zero free energy change, suggesting synergistic effects.

Conclusions:

  • The study provides crucial insights into the excellent HER activity of cobalt phosphide.
  • The findings highlight the importance of specific surface facets and synergistic effects of Co and P atoms for efficient HER.
  • This work lays a foundation for further mechanistic studies of HER on CoP and related transition-metal phosphides.