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<p>Atomic catalytic pairs (CPs) have shown great promise in driving multi-step catalytic transformations, yet the influence of spatial arrangement and coordination asymmetry on homonuclear CPs remain poorly understood. Herein, we construct atomically dispersed homonuclear Pt<sub>1</sub>-Pt<sub>1</sub> CPs with asymmetric Pt<sub>1</sub>C<sub>3</sub>-Pt<sub>1</sub>O<sub>1</sub>C<sub>3</sub> coordination anchored on reduced graphene oxide. By precisely tuning the spacing between the adjacent Pt<sub>1</sub>C<sub>3</sub>-Pt<sub>1</sub>O<sub>1</sub>C<sub>3</sub> CPs to approximately 5.3 Å, the catalyst achieves an exceptional turnover frequency of 27,218 h<sup>-1</sup> for transfer hydrogenation of azobenzene via ammonia-borane hydrolysis, surpassing benchmarking catalysts by more than an order of magnitude. The Pt<sub>1</sub>C<sub>3</sub>-Pt<sub>1</sub>O<sub>1</sub>C<sub>3</sub> CPs separated by 5.3 Å can facilitate co-adsorption of sterically hindered intermediates and at the same time the asymmetric Pt<sub>1</sub>C<sub>3</sub>-Pt<sub>1</sub>O<sub>1</sub>C<sub>3</sub> coordination enables facile hydrogen shuttling and barrier-suppressed hydrogenation. These synergistic effects enhance the overall azobenzene hydrogenation efficiency. Our findings uncover a fundamental spatial design principle for atomically precise homonuclear asymmetric CPs, offering new opportunities for sustainable and efficient fine chemical synthesis.</p>

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Asymmetric Pt1C3-Pt1O1C3 catalytic pairs for efficient transfer hydrogenation of azobenzene

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月2日

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  • Yiyun Fang,
  • Wen Zhao,
  • Zhilin Xing,
  • Cheng Chen,
  • Xin Zhou,
  • Congcong Cui,
  • Xuchao Wang,
  • Siming Zheng,
  • Qiyuan Liu,
  • Diandong Lv,
  • Siqi Li,
  • Zhaohang Chen,
  • Zi-Qiang Rong,
  • Na Guo,
  • Xinzhe Li,
  • Bin Liu

摘要

Atomic catalytic pairs (CPs) have shown great promise in driving multi-step catalytic transformations, yet the influence of spatial arrangement and coordination asymmetry on homonuclear CPs remain poorly understood. Herein, we construct atomically dispersed homonuclear Pt1-Pt1 CPs with asymmetric Pt1C3-Pt1O1C3 coordination anchored on reduced graphene oxide. By precisely tuning the spacing between the adjacent Pt1C3-Pt1O1C3 CPs to approximately 5.3 Å, the catalyst achieves an exceptional turnover frequency of 27,218 h-1 for transfer hydrogenation of azobenzene via ammonia-borane hydrolysis, surpassing benchmarking catalysts by more than an order of magnitude. The Pt1C3-Pt1O1C3 CPs separated by 5.3 Å can facilitate co-adsorption of sterically hindered intermediates and at the same time the asymmetric Pt1C3-Pt1O1C3 coordination enables facile hydrogen shuttling and barrier-suppressed hydrogenation. These synergistic effects enhance the overall azobenzene hydrogenation efficiency. Our findings uncover a fundamental spatial design principle for atomically precise homonuclear asymmetric CPs, offering new opportunities for sustainable and efficient fine chemical synthesis.