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Asymmetrically Coordinated Calcium Single Atom for High-Performance Oxygen Reduction Reaction.

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Calcium single atoms coordinated with sulfur, phosphorus, and nitrogen (Ca/NPS-HC) show superior performance for the oxygen reduction reaction (ORR). This novel catalyst design optimizes intermediate interactions, outperforming platinum-based catalysts.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • S-block single atoms are promising catalysts for the oxygen reduction reaction (ORR) due to their ability to suppress the Fenton reaction.
  • However, the inherent symmetry of s/p orbitals in S-block atoms often leads to suboptimal interactions with reaction intermediates, limiting catalytic efficiency.
  • Developing strategies to modulate these interactions is crucial for advancing S-block ORR catalysts.

Purpose of the Study:

  • To design and synthesize a novel S-block single-atom catalyst for enhanced ORR performance.
  • To modulate the adsorption of ORR intermediates through asymmetric coordination.
  • To investigate the underlying mechanism responsible for improved catalytic activity.

Main Methods:

  • Fabrication of calcium single atoms coordinated with sulfur (-S), phosphorus (-OP), and three nitrogen atoms (Ca/NPS-HC) on a high-carbon support.
  • Electrochemical evaluation of the Ca/NPS-HC catalyst for the oxygen reduction reaction (ORR).
  • Detailed mechanistic studies, including analysis of electron distribution and s-p hybridization, to elucidate the catalytic pathway.

Main Results:

  • The Ca/NPS-HC catalyst demonstrated exceptional ORR activity, achieving a half-wave potential of 0.89 V and a kinetic current density of 56.6 mA cm⁻² at 0.85 V.
  • The catalyst exhibited a low Tafel slope of 42 mV dec⁻¹, indicating efficient kinetics.
  • Performance surpassed that of commercial platinum on carbon (Pt/C) benchmarks.

Conclusions:

  • Asymmetric coordination of Ca single atoms in Ca/NPS-HC breaks the symmetry of electron distribution, leading to attenuated s-p hybridization during intermediate adsorption.
  • This modulation effectively minimizes the energy barrier for the overall ORR process.
  • The study presents a viable strategy for designing highly efficient S-block ORR catalysts by controlling intermediate adsorption through asymmetric coordination.