<p>Solid oxide fuel cells (SOFCs) enable direct and efficient conversion of transportable hydrocarbons into electricity, offering a scalable pathway for carbon-neutral energy systems. A critical challenge in SOFC development lies in the atomic-scale structural regulation of perovskite-type anodes, which is essential for enhancing hydrocarbon oxidation kinetics while mitigating carbon deposition issues. To overcome this fundamental limitation, we propose an entropy-driven strategy to induce order-to-disorder transitions in perovskite oxides. This strategy is demonstrated in the layered ordered perovskite PrBaFe<sub>2</sub>O<sub>5+δ</sub>, where the introduction of five equimolar rare-earth cations at the Pr site results in the formation of a disordered A-site high-entropy perovskite anode with the composition La<sub>0.2</sub>Pr<sub>0.2</sub>Sm<sub>0.2</sub>Gd<sub>0.2</sub>Y<sub>0.2</sub>BaFe<sub>2</sub>O<sub>5+δ</sub> (HEP). Such atomic-scale order-to-disorder transitions facilitate oxygen vacancy formation and improve anode hydration capacity, thereby accelerating both hydrocarbon steam reforming and carbon elimination processes. The designed HEP anode exhibits a peak power density of 774.53 mW·cm<sup>–2</sup> and stability over 1000 hours under wet methane (3 vol% H<sub>2</sub>O) at 700 °C. The present work contributes a new strategy for controlling ion ordering in perovskite oxides, addressing key challenges in SOFC operating with hydrocarbon fuels.</p>

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Entropy-driven order-to-disorder transition in perovskite anodes for high-performance solid oxide fuel cells

  • Gaige Wang,
  • Rongzheng Ren,
  • Xiaodan Yu,
  • Chunming Xu,
  • Jinshuo Qiao,
  • Wang Sun,
  • Zhenhua Wang,
  • Kening Sun

摘要

Solid oxide fuel cells (SOFCs) enable direct and efficient conversion of transportable hydrocarbons into electricity, offering a scalable pathway for carbon-neutral energy systems. A critical challenge in SOFC development lies in the atomic-scale structural regulation of perovskite-type anodes, which is essential for enhancing hydrocarbon oxidation kinetics while mitigating carbon deposition issues. To overcome this fundamental limitation, we propose an entropy-driven strategy to induce order-to-disorder transitions in perovskite oxides. This strategy is demonstrated in the layered ordered perovskite PrBaFe2O5+δ, where the introduction of five equimolar rare-earth cations at the Pr site results in the formation of a disordered A-site high-entropy perovskite anode with the composition La0.2Pr0.2Sm0.2Gd0.2Y0.2BaFe2O5+δ (HEP). Such atomic-scale order-to-disorder transitions facilitate oxygen vacancy formation and improve anode hydration capacity, thereby accelerating both hydrocarbon steam reforming and carbon elimination processes. The designed HEP anode exhibits a peak power density of 774.53 mW·cm–2 and stability over 1000 hours under wet methane (3 vol% H2O) at 700 °C. The present work contributes a new strategy for controlling ion ordering in perovskite oxides, addressing key challenges in SOFC operating with hydrocarbon fuels.