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<p>The unique catalytic activity of small nanoparticles can be attributed to their distinctive electronic structure and/or their ability to expose sites with a unique geometry. Quantifying and distinguishing the contributions of these effects to catalytic performance presents a challenge, given the complexity arising from multiple influencing factors and the lack of a quantitative structure-activity relationship. Here, we show that the intrinsic activity of platinum atoms at the perimeter corner sites is three orders of magnitude higher as a result of an electronic structure effect, with a threshold occurring at an average nanoparticle size of 1-1.5 nm. The contributions to the activity of atomically dispersed platinum, large nanoparticles and sodium-induced support modification are minor. This comprehensive and quantitative structure-activity correlation was demonstrated and verified on real-world Pt/CeO<sub>2</sub> catalysts for the water-gas shift reaction by utilizing operando X-ray photoelectron spectroscopy, in situ scanning transmission electron microscopy, electron energy-loss spectroscopy, theoretical calculations, and kinetic models.</p>

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Quantifying electronic and geometric effects on the activity of platinum catalysts for water-gas shift

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年7月18日

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  • Xiansheng Li,
  • Xing Wang,
  • Arik Beck,
  • Mikalai Artsiusheuski,
  • Qianyu Liu,
  • Qiang Liu,
  • Henrik Eliasson,
  • Frank Krumeich,
  • Ulrich Aschauer,
  • Giovanni Pizzi,
  • Rolf Erni,
  • Jeroen A. van Bokhoven,
  • Luca Artiglia

摘要

The unique catalytic activity of small nanoparticles can be attributed to their distinctive electronic structure and/or their ability to expose sites with a unique geometry. Quantifying and distinguishing the contributions of these effects to catalytic performance presents a challenge, given the complexity arising from multiple influencing factors and the lack of a quantitative structure-activity relationship. Here, we show that the intrinsic activity of platinum atoms at the perimeter corner sites is three orders of magnitude higher as a result of an electronic structure effect, with a threshold occurring at an average nanoparticle size of 1-1.5 nm. The contributions to the activity of atomically dispersed platinum, large nanoparticles and sodium-induced support modification are minor. This comprehensive and quantitative structure-activity correlation was demonstrated and verified on real-world Pt/CeO2 catalysts for the water-gas shift reaction by utilizing operando X-ray photoelectron spectroscopy, in situ scanning transmission electron microscopy, electron energy-loss spectroscopy, theoretical calculations, and kinetic models.