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Tuning Exsolution and Surface Properties via Excess Free Energy and Work Function Engineering for High-Performance

Bingbing Qiu1, Zohaib Ur Rehman1, Kang Zhu1

  • 1Department of Materials Science and Engineering, University of Science and Technology of China, 96 Jinzhai Road, Hefei, Anhui 230026, China.

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|June 9, 2026
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Summary
This summary is machine-generated.

Doping La$_{0.5}$Ba$_{0.5}$Co$_{0.4}$Fe$_{0.6}$O$_{3-δ}$ (LBCF) with cerium (Ce) promotes nanoparticle exsolution, significantly boosting protonic ceramic fuel cell performance. This engineered cathode design enhances the oxygen reduction reaction, achieving a 87% power density improvement.

Keywords:
Gibbs free energyaccumulation layerexsolutionoxygen reduction reactionphase separationwork function

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Nanoparticle exsolution is a key strategy for improving surface-mediated oxygen reduction reactions (p-ORR) in protonic ceramic fuel cells.
  • Thermodynamic drivers and the exact function of exsolved nanoparticles in LBCF cathodes are not fully understood.

Purpose of the Study:

  • To investigate the exsolution behavior of B-site doped LBCF (Ce, Pr, Zr, Sn) and its impact on p-ORR.
  • To establish a predictive framework linking dopant thermodynamics, exsolution, and catalytic activity for rational cathode design.

Main Methods:

  • Density functional theory (DFT) calculations to determine excess Gibbs free energy of exsolution (ΔGex).
  • Experimental synthesis and characterization of doped LBCF materials.
  • Work function analysis and temperature-programmed desorption (CO2/NH3-TPD) to study surface interactions.

Main Results:

  • DFT predicted ΔGex accurately correlates with experimental exsolution behavior: Ce- and Pr-doped LBCF exsolved nanoparticles, while Zr- and Sn-doped LBCF remained single-phase.
  • Exsolved BaCeO3 nanoparticles on Ce-doped LBCF enhanced electron transfer and surface oxygen exchange.
  • Ce-doped LBCF cathodes demonstrated significantly lower polarization resistance and higher oxygen surface exchange coefficients.

Conclusions:

  • The study successfully links dopant thermodynamics to nanoparticle exsolution and catalytic performance in LBCF cathodes.
  • Ce-doped LBCF cathodes achieved a peak power density of 0.97 W cm⁻² at 650 °C, an 87% improvement over pristine LBCF.
  • This work provides a predictive framework for designing advanced exsolution-engineered cathodes for fuel cells.