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<p>Single-atom catalysts (SACs) have attracted significant interest due to their exceptional and tunable performance, enabled by diverse coordination environments achieved through innovative synthetic strategies. However, various local structures of active sites pose significant challenges for precise characterization, a prerequisite for developing structure-activity relationships. Here, we combine <sup>17</sup>O solid-state NMR spectroscopy and DFT calculations to elucidate the detailed structural information of Pt/CeO<sub>2</sub> SACs and their catalytic behaviors. The NMR data reveal that single Pt atoms, dispersed from clusters with water vapor, exhibit a square planar geometry embedded in CeO<sub>2</sub> (111) surface, distinct from the original clusters and other conventionally generated Pt single atoms. The square planar Pt/CeO<sub>2</sub> SAC demonstrates improved CO oxidation performance compared to Pt/CeO<sub>2</sub> SAC with octahedral coordination, due to moderately strong CO adsorption and low energy barriers. This approach can be extended to other oxide-supported SACs, enabling spatially resolved characterization and offering comprehensive insights into their structure-activity relationships.</p>

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Revealing the structure-activity relationship of Pt1/CeO2 with 17O solid-state NMR spectroscopy and DFT calculations

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月14日

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  • Yujie Wen,
  • Fang Wang,
  • Jie Zhu,
  • Qian Wen,
  • Xiaoli Xia,
  • Juan Wen,
  • Changshun Deng,
  • Jia-Huan Du,
  • Xiaokang Ke,
  • Zhen Zhang,
  • Hanxi Guan,
  • Lei Nie,
  • Meng Wang,
  • Wenhua Hou,
  • Wei Li,
  • Weiping Tang,
  • Weiping Ding,
  • Junchao Chen,
  • Luming Peng

摘要

Single-atom catalysts (SACs) have attracted significant interest due to their exceptional and tunable performance, enabled by diverse coordination environments achieved through innovative synthetic strategies. However, various local structures of active sites pose significant challenges for precise characterization, a prerequisite for developing structure-activity relationships. Here, we combine 17O solid-state NMR spectroscopy and DFT calculations to elucidate the detailed structural information of Pt/CeO2 SACs and their catalytic behaviors. The NMR data reveal that single Pt atoms, dispersed from clusters with water vapor, exhibit a square planar geometry embedded in CeO2 (111) surface, distinct from the original clusters and other conventionally generated Pt single atoms. The square planar Pt/CeO2 SAC demonstrates improved CO oxidation performance compared to Pt/CeO2 SAC with octahedral coordination, due to moderately strong CO adsorption and low energy barriers. This approach can be extended to other oxide-supported SACs, enabling spatially resolved characterization and offering comprehensive insights into their structure-activity relationships.