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<p>Dual-atom catalysts (DACs) represent a frontier in heterogeneous electrocatalysis for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. However, the dynamic evolution of active-site structure complicates mechanistic understanding. Herein, alloyed Fe-Co DACs with strong Fe-Co bonds are synthesized via molecular chelation and ionic coupling strategies. In-situ spectroscopy combined with theoretical calculation reveals the Janus effect of Fe-Co dual-atom sites: Co serves as the primary catalytic center for the 4e<sup>-</sup> process with Fe as the cooperative sites to absorb the *OH. This division-of-labor mechanism lowers the theoretical overpotential from 1.14 V to 0.43 V for acidic oxygen reduction reaction. Thus, the catalyst achieves a 0.852 V half-wave potential and 1.14 W cm<sup>−2</sup> power density (2.0 bar H₂-O₂), sustaining 81% peak power after 10,000 cycles. These findings clarify DAC configuration-mechanism relationships, guiding the design of high-performance DACs.</p>

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Janus effect of FeCo dual atom catalyst with Co as active center in acidic oxygen reduction reaction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月5日

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  • Long-Ji Yuan,
  • Zhen-Yu Miao,
  • Xu-Lei Sui,
  • Chi-Feng Lee,
  • Qi Li,
  • Mei-Jie Yin,
  • Li-Xiao Shen,
  • Ying-Rui Lu,
  • Zi-Gang Zhao,
  • Yu-Zhe Liu,
  • Lin-Sheng Zhu,
  • Wei Gong,
  • Wen-Liang Feng,
  • Hsiao-Tsu Wang,
  • Guo-Xu Zhang,
  • Zhen-Bo Wang

摘要

Dual-atom catalysts (DACs) represent a frontier in heterogeneous electrocatalysis for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. However, the dynamic evolution of active-site structure complicates mechanistic understanding. Herein, alloyed Fe-Co DACs with strong Fe-Co bonds are synthesized via molecular chelation and ionic coupling strategies. In-situ spectroscopy combined with theoretical calculation reveals the Janus effect of Fe-Co dual-atom sites: Co serves as the primary catalytic center for the 4e- process with Fe as the cooperative sites to absorb the *OH. This division-of-labor mechanism lowers the theoretical overpotential from 1.14 V to 0.43 V for acidic oxygen reduction reaction. Thus, the catalyst achieves a 0.852 V half-wave potential and 1.14 W cm−2 power density (2.0 bar H₂-O₂), sustaining 81% peak power after 10,000 cycles. These findings clarify DAC configuration-mechanism relationships, guiding the design of high-performance DACs.