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Thermodynamically and Kinetically Stabilized Pt Clusters Against Sintering on CeO 2 Nanofibers Through Enclosing CeO 2 Nanocubes.

Jun WangSuting LiuMingyu TangWanlin FuYunpeng WangKuibo YinYun-Qian Dai
Published in: Small (Weinheim an der Bergstrasse, Germany) (2023)
Sintering is a major concern for the deactivation of supported metals catalysts, which is driven by the force of decreasing the total surface energy of the entire catalytic system. In this work, a double-confinement strategy is demonstrated to stabilize 2.6 nm-Pt clusters against sintering on electrospun CeO 2 nanofibers decorated by CeO 2 nanocubes (m-CeO 2 ). Thermodynamically, with the aid of CeO 2 -nanocubes, the intrinsically irregular surface of polycrystalline CeO 2 nanofibers becomes smooth, offering adjacent Pt clusters with decreased chemical potential differences on a relatively uniform surface. Kinetically, the Pt clusters are physically restricted on each facet of CeO 2 nanocubes in a nanosized region. In situ high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) observation reveals that the Pt clusters can be stabilized up to 800 °C even in a high density, which is far beyond their Tammann temperature, without observable size growth or migration. Such a sinter-resistant catalytic system is endowed with boosted catalytic activity toward both the hydrogenation of p-nitrophenol after being aged at 500 °C and the sinter-promoting exothermic oxidation reactions (e.g., soot oxidation) at high temperatures over 700 °C. This work offers new opportunities for exploring sinter-resistant nanocatalysts, starting from the rational design of whole catalytic system in terms of thermodynamic and kinetic aspects.
Keyphrases
  • electron microscopy
  • high density
  • high resolution
  • hydrogen peroxide
  • highly efficient
  • mass spectrometry
  • risk assessment
  • photodynamic therapy
  • health risk
  • health risk assessment