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Dynamic Evolution of Solid-Liquid Electrochemical Interfaces over Single-Atom Active Sites.

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  • 1National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, Anhui P. R. China.

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Summary
This summary is machine-generated.

Single-atom nickel catalysts dynamically evolve at solid-liquid interfaces during the oxygen reduction reaction (ORR), forming isolated active sites for highly efficient catalysis in alkaline solutions.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Surface Chemistry

Background:

  • Structural dynamics at solid-liquid interfaces (SLEIs) are crucial for electrochemical processes.
  • Understanding atomic-level transformations is key to designing efficient catalysts.

Purpose of the Study:

  • To investigate the atomic-level structural dynamics of single-atom nickel (Ni) at SLEIs during the oxygen reduction reaction (ORR).
  • To elucidate the formation and role of active sites in enhancing ORR performance.

Main Methods:

  • Operando synchrotron spectroscopies were employed to study atomic-level structural dynamics.
  • Combined spectroscopic techniques provided in-situ insights into catalyst evolution.

Main Results:

  • Single-atom Ni at SLEIs evolves into a near-free atom state during the ORR.
  • A dynamic release from the substrate forms isolated-zigzag active sites (Ni1(2-δ)+N2).
  • These active sites efficiently adsorb and dissociate O2, forming key intermediates.

Conclusions:

  • The identified isolated-zigzag Ni active sites significantly enhance ORR performance in alkaline media.
  • This work offers a general approach to study dynamic processes at SLEIs for various electrochemical reactions.