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<p>Interfacial oxygen migration from support to noble metal active sites, termed reverse oxygen spillover, represents a critical metal-support interaction influencing the performance of Pt/TiO<sub>2</sub> catalysts. In this study, we uncover a size effect of Pt particles on reverse oxygen spillover in Pt/Sn<sub>0.2</sub>Ti<sub>0.8</sub>O<sub>2</sub> catalysts via a combination of in situ characterizations with ab initio molecular dynamics simulations. Among single-atom Pt, nanocluster Pt, and nanocrystal Pt, nanocluster Pt exhibits the most pronounced reverse oxygen spillover and thus achieves the highest turnover frequency in CO oxidation. The most pronounced reverse oxygen spillover is mainly due to the strongest electron transfer to the interfacial lattice oxygen triggered by CO adsorption with moderate adsorption energy. In contrast, CO adsorption on single-atom Pt is too strong to initiate reverse oxygen spillover, while on nanocrystal Pt, it leads to a weakening of the interaction between Pt sites and the support, thus hinders the reverse oxygen spillover. This study clarifies the relationship between Pt particle size and reverse oxygen spillover effects, furnishing a theoretical basis for designing noble metal catalysts with excellent activity.</p>

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Pt size-dependent reverse oxygen spillover on Sn-doped Pt/TiO2 for CO oxidation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月3日

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  • Shangchao Xiong,
  • Zhengjun Gong,
  • Houlin Wang,
  • Jianqiang Shi,
  • Haiyan Liu,
  • Xiaoping Chen,
  • Jinxing Mi,
  • Jianjun Chen,
  • Junhua Li

摘要

Interfacial oxygen migration from support to noble metal active sites, termed reverse oxygen spillover, represents a critical metal-support interaction influencing the performance of Pt/TiO2 catalysts. In this study, we uncover a size effect of Pt particles on reverse oxygen spillover in Pt/Sn0.2Ti0.8O2 catalysts via a combination of in situ characterizations with ab initio molecular dynamics simulations. Among single-atom Pt, nanocluster Pt, and nanocrystal Pt, nanocluster Pt exhibits the most pronounced reverse oxygen spillover and thus achieves the highest turnover frequency in CO oxidation. The most pronounced reverse oxygen spillover is mainly due to the strongest electron transfer to the interfacial lattice oxygen triggered by CO adsorption with moderate adsorption energy. In contrast, CO adsorption on single-atom Pt is too strong to initiate reverse oxygen spillover, while on nanocrystal Pt, it leads to a weakening of the interaction between Pt sites and the support, thus hinders the reverse oxygen spillover. This study clarifies the relationship between Pt particle size and reverse oxygen spillover effects, furnishing a theoretical basis for designing noble metal catalysts with excellent activity.