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<p>Heterogeneous dual-atom catalysts (DACs) offer great potential to enhance electrocatalytic reaction kinetics and provide diverse active sites. However, achieving precise tuning of metal atom coordination in DACs remains a significant challenge. Here, the axial dual atom (ADA) embedded within a covalent organic framework and N-doped graphene, features an axial intermetallic distance tuned by alcohol solvent treatment, resulting in efficient bifunctional electrocatalysis of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). In situ X-ray absorption near-edge spectroscopy (XANES) and Raman spectroscopy reveal that Fe acts as the primary active center in the axially coordinated FeCo-ADA, with Co providing synergistic effects. The in-depth theoretical analysis elucidates that the axial Fe-Co orbital coupling results in optimized orbital energy levels, higher Fe oxidation state, weakened oxygen intermediate binding strength, and reduced reaction energy barrier. The zinc-air battery (ZAB) equipped with FeCo-ADA achieves a high peak power density of 464.5 mW cm<sup>-2</sup> and exhibits long rechargeability of 3710 hours at 10 mA cm<sup>-2</sup>. Our findings pave an avenue for the rational design in axial DACs to enhance the electrocatalytic performance for energy conversion.</p>

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Spatial engineering and d-orbital coupling in axial dual-atom sites for bifunctional oxygen catalysis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月16日

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  • Xinru Yan,
  • Xiaoliang Yuan,
  • Ning Liu,
  • Bin Liao,
  • Zhanhao Liang,
  • Wencai Liu,
  • Yihui Huang,
  • Longwen Yan,
  • Qing Zheng,
  • Shufen Chen,
  • Xi Xie,
  • Xuchun Gui,
  • Hong Bin Yang,
  • Jiling Li,
  • Dingshan Yu,
  • Zhiping Zeng,
  • Guowei Yang

摘要

Heterogeneous dual-atom catalysts (DACs) offer great potential to enhance electrocatalytic reaction kinetics and provide diverse active sites. However, achieving precise tuning of metal atom coordination in DACs remains a significant challenge. Here, the axial dual atom (ADA) embedded within a covalent organic framework and N-doped graphene, features an axial intermetallic distance tuned by alcohol solvent treatment, resulting in efficient bifunctional electrocatalysis of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). In situ X-ray absorption near-edge spectroscopy (XANES) and Raman spectroscopy reveal that Fe acts as the primary active center in the axially coordinated FeCo-ADA, with Co providing synergistic effects. The in-depth theoretical analysis elucidates that the axial Fe-Co orbital coupling results in optimized orbital energy levels, higher Fe oxidation state, weakened oxygen intermediate binding strength, and reduced reaction energy barrier. The zinc-air battery (ZAB) equipped with FeCo-ADA achieves a high peak power density of 464.5 mW cm-2 and exhibits long rechargeability of 3710 hours at 10 mA cm-2. Our findings pave an avenue for the rational design in axial DACs to enhance the electrocatalytic performance for energy conversion.