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<p>Protonic ceramic fuel cells (PCFCs) operating on NH<sub>3</sub> present a promising carbon-free energy pathway, yet their performance is often constrained by limited catalytic activity and degradation of conventional Ni-based anodes. Here, we report a high-entropy perovskite catalyst, Sr<sub>2</sub>Fe<sub>1</sub>Mo<sub>0.2</sub>Mn<sub>0.2</sub>Cr<sub>0.2</sub>Cu<sub>0.2</sub>Ni<sub>0.2</sub>O<sub>6-<i>δ</i></sub> (SFMMCCN), employed as an anode catalyst layer in direct ammonia-fed PCFCs. Upon reduction, SFMMCCN undergoes in situ exsolution of Ni–Fe–Cu alloy nanoparticles within a stable oxide matrix. This architecture provides synergistic enhancement of NH<sub>3</sub> adsorption and decomposition through the combined effects of abundant surface acid sites and catalytically active alloy interfaces. As a result, the SFMMCCN cell achieves a record peak power density of 2.04 W&#xa0;cm⁻<sup>2</sup> at 700&#xa0;°C and demonstrates excellent operational stability for over 255&#xa0;h at 600&#xa0;°C under NH<sub>3</sub> fuel. Compared to a bare cell, it exhibits significantly reduced polarization resistance and effectively suppresses Ni coarsening. Density functional theory calculations reveal that the high-entropy oxide framework, together with the exsolved Ni–Fe–Cu alloy, lowers the energy barriers for NH<sub>3</sub> decomposition, thereby accelerating overall catalytic kinetics. These findings highlight entropy-controlled oxide–metal architectures as a powerful strategy to achieve both high performance and durability in NH<sub>3</sub>-fueled electrochemical systems, offering a viable pathway toward scalable and efficient hydrogen-based power generation.</p>

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Entropy-Modulated Oxide–Metal Catalyst Architectures for Direct Ammonia Protonic Ceramic Fuel Cells

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年4月17日

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  • Dongyeon Kim,
  • Dong Jae Park,
  • Incheol Jeong,
  • Seeun Oh,
  • Hyeonggeun Kim,
  • Mincheol Lee,
  • Sang Won Lee,
  • Kangyong Lee,
  • Daehan Chung,
  • Ki-Min Roh,
  • Joongmyeon Bae,
  • Tae Ho Shin,
  • Kang Taek Lee

摘要

Protonic ceramic fuel cells (PCFCs) operating on NH3 present a promising carbon-free energy pathway, yet their performance is often constrained by limited catalytic activity and degradation of conventional Ni-based anodes. Here, we report a high-entropy perovskite catalyst, Sr2Fe1Mo0.2Mn0.2Cr0.2Cu0.2Ni0.2O6-δ (SFMMCCN), employed as an anode catalyst layer in direct ammonia-fed PCFCs. Upon reduction, SFMMCCN undergoes in situ exsolution of Ni–Fe–Cu alloy nanoparticles within a stable oxide matrix. This architecture provides synergistic enhancement of NH3 adsorption and decomposition through the combined effects of abundant surface acid sites and catalytically active alloy interfaces. As a result, the SFMMCCN cell achieves a record peak power density of 2.04 W cm⁻2 at 700 °C and demonstrates excellent operational stability for over 255 h at 600 °C under NH3 fuel. Compared to a bare cell, it exhibits significantly reduced polarization resistance and effectively suppresses Ni coarsening. Density functional theory calculations reveal that the high-entropy oxide framework, together with the exsolved Ni–Fe–Cu alloy, lowers the energy barriers for NH3 decomposition, thereby accelerating overall catalytic kinetics. These findings highlight entropy-controlled oxide–metal architectures as a powerful strategy to achieve both high performance and durability in NH3-fueled electrochemical systems, offering a viable pathway toward scalable and efficient hydrogen-based power generation.