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<p>Development of efficient and durable oxygen reduction reaction (ORR) electrocatalysts is of great interest yet remains challenging. Herein, we predicted and screened a bilayer graphite carbon-supported Ir-N<sub>4</sub>/Fe-N<sub>4</sub> catalyst with high ORR activity using density functional theory calculations. Subsequently, various bimetallic single atom supported on 3D ordered macroporous carbon were rationally designed and experimentally synthesized via a colloidal microsphere template-confined reaction method. As anticipated, the resulting Ir-N<sub>4</sub>/Fe-N<sub>4</sub> bimetallic single-atom catalysts (IrFe-SACs) exhibit superior ORR activity and durability, reaching a half-wave potential of 0.928&#xa0;V. The IrFe-SACs also demonstrate outstanding performance in Zn-air batteries, including a high discharge power density (314&#xa0;mW cm⁻<sup>2</sup>) and excellent cycling stability (~ 1650 cycles over 550&#xa0;h). Further experimental characterizations and theoretical analysis reveal that introducing interlayer-adjacent Ir-N<sub>4</sub> sites facilitates the transition of Fe-N<sub>4</sub> from a low-spin state to a medium-spin state, which optimizes the spin polarization of Fe 3d orbitals and enhances the non-localization of the Fe–O/OH molecular orbital, thereby significantly improving the ORR intrinsic activity and durability of atomic Fe-N<sub>4</sub> sites. </p>

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Modulation of the Spin State of Atomic Fe-N4 Sites with Interlayer-Adjacent Ir-N4 for Superior ORR Activity

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月5日

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  • Yan Tan,
  • Aoshuang Li,
  • Yijie Wang,
  • Xiucai Jiang,
  • Yiwen Cheng,
  • Dongliang Chao,
  • Yuzhong Zhang,
  • Chuanwei Cheng

摘要

Development of efficient and durable oxygen reduction reaction (ORR) electrocatalysts is of great interest yet remains challenging. Herein, we predicted and screened a bilayer graphite carbon-supported Ir-N4/Fe-N4 catalyst with high ORR activity using density functional theory calculations. Subsequently, various bimetallic single atom supported on 3D ordered macroporous carbon were rationally designed and experimentally synthesized via a colloidal microsphere template-confined reaction method. As anticipated, the resulting Ir-N4/Fe-N4 bimetallic single-atom catalysts (IrFe-SACs) exhibit superior ORR activity and durability, reaching a half-wave potential of 0.928 V. The IrFe-SACs also demonstrate outstanding performance in Zn-air batteries, including a high discharge power density (314 mW cm⁻2) and excellent cycling stability (~ 1650 cycles over 550 h). Further experimental characterizations and theoretical analysis reveal that introducing interlayer-adjacent Ir-N4 sites facilitates the transition of Fe-N4 from a low-spin state to a medium-spin state, which optimizes the spin polarization of Fe 3d orbitals and enhances the non-localization of the Fe–O/OH molecular orbital, thereby significantly improving the ORR intrinsic activity and durability of atomic Fe-N4 sites.