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Activity and stability origin of core-shell catalysts: unignorable atomic diffusion behavior.

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Core-shell catalysts show excellent oxygen reduction and evolution reactions. Dynamic structural evolution, including atomic diffusion, is key to the activity and long-term stability of these electrocatalysts.

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Area of Science:

  • Electrocatalysis
  • Materials Science
  • Surface Chemistry

Background:

  • Core-shell catalysts exhibit promising performance in oxygen reduction reaction (ORR) and oxygen evolution reaction (OER).
  • Understanding the origins of their activity and durability typically relies on static structural analysis, potentially overlooking dynamic processes.

Purpose of the Study:

  • To elucidate the active structure and stability mechanisms of NiFe@NC core-shell catalysts for ORR and OER.
  • To investigate the role of dynamic structural evolution in electrocatalyst performance and longevity.

Main Methods:

  • Utilized a NiFe alloy coated with a nitrogen-doped carbon shell (NiFe@NC) as a model system.
  • Combined constant potential computations, *ab initio* molecular dynamics simulations, and experimental validation.
  • Analyzed atomic diffusion behaviors during electrochemical reactions.

Main Results:

  • Synergistic effects between the alloy core and carbon shell promote Fe-N-C active site formation.
  • The core acts as a reservoir, replenishing metal sites and ensuring long-term stability.
  • Atomic diffusion is critical for the dynamic formation and regeneration of active sites during ORR/OER.

Conclusions:

  • Dynamic structural evolution and reconstruction are crucial for the high activity and stability of core-shell electrocatalysts.
  • The 'ammunition depot' and 'automatic loader' analogy highlights the interplay between the core and shell for sustained performance.
  • This study provides fundamental insights into designing robust and efficient electrocatalysts for energy applications.