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<p>Precisely identifying the atomic structure of reducible oxide-supported metal clusters remains challenging yet critical for understanding their catalytic behavior. Herein, we report the preparation of CeO<sub>2</sub>-supported bi-layer Pt clusters (Pt<sub><i>n</i></sub>/CeO<sub>2</sub>) via a deposition-reduction strategy, with Pt cluster sizes ranging from 0.8 to 1.2 nm (9–30 atoms). Through combined aberrationcorrected high-angle annular dark field scanning transmission electron microscope (HAADF-STEM) imaging, quantitative STEM simulations, and X-ray fine structure (XAFS) analysis, we reveal the bi-layer configuration featuring coordinatively unsaturated Pt<sup>0</sup> sites on the top layer while maintaining Pt-CeO<sub>2</sub> interfacial bonding at the bottom. When applied to anti-Markovnikov alkene hydrosilylation, Pt<sub><i>n</i></sub>/CeO<sub>2</sub> achieves 99.9% silane conversion with a mass-specific activity 2.0× and 8.8× higher than single-atom site (Pt<sub>1</sub>/CeO<sub>2</sub>) and nanoparticle (Pt<sub>NP</sub>/CeO<sub>2</sub>) counterparts, respectively. The bi-layer structure endows exceptional cycling stability and anti-leaching properties. This work establishes a multi-scale characterization paradigm to resolve atomic-precision structures of supported clusters, opening avenues for designing robust catalysts with tailored metaloxide interfaces.</p>

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CeO2-supported bi-layer Pt clusters for anti-Markovnikov alkene hydrosilylation

  • 期刊论文

  • 发表日期：

    2025年8月7日

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  • Sunpei Hu,
  • Haofan Lei,
  • Junlong Shi,
  • Yongjie Ye,
  • Fenglin Peng,
  • Wenlong Wu,
  • Jian Zhang,
  • Han Yan,
  • Chao Ma,
  • Jie Zeng

摘要

Precisely identifying the atomic structure of reducible oxide-supported metal clusters remains challenging yet critical for understanding their catalytic behavior. Herein, we report the preparation of CeO2-supported bi-layer Pt clusters (Ptn/CeO2) via a deposition-reduction strategy, with Pt cluster sizes ranging from 0.8 to 1.2 nm (9–30 atoms). Through combined aberrationcorrected high-angle annular dark field scanning transmission electron microscope (HAADF-STEM) imaging, quantitative STEM simulations, and X-ray fine structure (XAFS) analysis, we reveal the bi-layer configuration featuring coordinatively unsaturated Pt0 sites on the top layer while maintaining Pt-CeO2 interfacial bonding at the bottom. When applied to anti-Markovnikov alkene hydrosilylation, Ptn/CeO2 achieves 99.9% silane conversion with a mass-specific activity 2.0× and 8.8× higher than single-atom site (Pt1/CeO2) and nanoparticle (PtNP/CeO2) counterparts, respectively. The bi-layer structure endows exceptional cycling stability and anti-leaching properties. This work establishes a multi-scale characterization paradigm to resolve atomic-precision structures of supported clusters, opening avenues for designing robust catalysts with tailored metaloxide interfaces.