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Blocking the Operando Formation of Single-Atom Spectators by Interfacial Engineering.

Xuan Tang1,2,3, Shasha Ge1, Yao Lv1,2

  • 1State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, P.R. China.

Angewandte Chemie (International Ed. in English)
|April 3, 2025
PubMed
Summary

Catalyst deactivation in propane oxidation is caused by platinum (Pt) nanoclusters dispersing into unreactive single atoms. Introducing niobium oxide (NbOx) prevents this, significantly boosting catalyst performance.

Keywords:
AntidispersionBlocking effectCatalyst deactivationHeterogeneous catalysisInterfacial engineering

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Area of Science:

  • Heterogeneous catalysis
  • Materials science
  • Surface chemistry

Background:

  • Catalyst stability is crucial for heterogeneous catalysis, with sintering traditionally blamed for deactivation.
  • The Pt/CeO2 catalyst shows reduced activity in complete propane oxidation at low temperatures.
  • This deactivation is linked to platinum (Pt) nanoclusters dispersing into less reactive single atoms under reaction conditions.

Purpose of the Study:

  • To investigate the mechanism of Pt/CeO2 catalyst deactivation in propane oxidation.
  • To develop a strategy to enhance the stability and activity of Pt/CeO2 catalysts.
  • To understand the role of surface engineering in preventing the formation of inactive single-atom sites.

Main Methods:

  • Operando characterization of Pt/CeO2 catalysts during complete propane oxidation.
  • Surface modification of CeO2 support with niobium oxide (NbOx).
  • Comparative activity testing of engineered and conventional catalysts.

Main Results:

  • Loss of activity in Pt/CeO2 is due to Pt nanocluster dispersion into spectator single atoms.
  • Engineered NbOx on CeO2 prevents Pt redispersion and preserves active Pt ensembles.
  • The NbOx-modified catalyst exhibited a 37-fold increase in reaction rate compared to unmodified Pt/CeO2.

Conclusions:

  • Suppression of noble metal single-atom spectator formation via surface engineering is vital for catalyst performance.
  • Mechanistic insights into Pt/CeO2 deactivation advance materials science.
  • Findings have implications for energy conversion and environmental remediation technologies.