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U2O5 Film Preparation via UO2 Deposition by Direct Current Sputtering and Successive Oxidation and Reduction with Atomic Oxygen and Atomic Hydrogen
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High-valence Ir single atoms enhance oxygen evolution electrocatalysis.

Runxin Li1, Yangyang Dong1, Heng Xu2

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Synthesizing stable high-valent single-atom catalysts is challenging. This study developed a method to stabilize iridium single atoms on a nickel sulfide matrix, achieving excellent oxygen evolution reaction (OER) performance.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • High-valent metal single atoms offer superior electrocatalytic activity due to fast electron transfer.
  • Synthesizing these catalysts is difficult because they are unstable under standard preparation conditions.

Purpose of the Study:

  • To develop a robust strategy for synthesizing stable high-valent single-atom catalysts.
  • To investigate the electrocatalytic performance of atomically dispersed Ir3+ single atoms on a NiS2 matrix for the oxygen evolution reaction (OER).

Main Methods:

  • Atomically dispersed Ir3+ single atoms were synthesized by substituting Ni lattice sites in NiS2 with Ir.
  • Coordination with adjacent sulfur atoms stabilized the Ir species.
  • Density-functional theory (DFT) calculations were employed to understand the electronic structure and catalytic mechanism.

Main Results:

  • The synthesized catalyst demonstrated outstanding OER performance, reaching a current density of 10 mA cm-2 at a low overpotential of 190 mV.
  • DFT calculations indicated that the high oxidation state of Ir shifts the Ni d-band center, enhancing OOH* adsorption and accelerating OER kinetics.
  • The NiS2 sulfide support proved effective in stabilizing the high oxidation state of iridium.

Conclusions:

  • A reliable method for constructing stable high-valent single-atom catalysts was established.
  • The study highlights the crucial role of sulfide supports in stabilizing high oxidation states for advanced electrocatalysis.
  • The developed catalyst shows significant potential for efficient oxygen evolution reactions.