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Area of Science:

  • Catalysis
  • Surface Science
  • Materials Science

Background:

  • Operando catalysis studies are crucial for industrial catalyst development.
  • Previous operando X-ray photoelectron spectroscopy (XPS) experiments were limited to low pressures, questioning their industrial relevance.

Purpose of the Study:

  • To perform fundamental operando catalysis studies under industrially relevant conditions.
  • To investigate carbon monoxide oxidation on Pd(100) at 1 bar using XPS.
  • To analyze the surface chemical composition and kinetics at the atomistic level.

Main Methods:

  • Operando X-ray photoelectron spectroscopy (XPS) at 1 bar total pressure.
  • Utilized hard X-rays and a grazing incident angle for high-pressure and surface sensitivity.
  • In situ oxidation study at 70 mbar to confirm surface sensitivity and peak assignments.

Main Results:

  • Successfully monitored CO oxidation on Pd(100) at 1 bar, observing gas-phase photoemission peaks for CO2, CO, and O2.
  • Determined reaction kinetics and calculated activation energy during the light-off regime.
  • Identified a metallic Pd phase in the highly active regime, with no oxygen-induced peaks observed during reaction.

Conclusions:

  • Demonstrated the capability of operando XPS with hard X-rays for high-pressure catalysis studies.
  • Achieved atomistic chemical information of catalysts under industrially relevant conditions.
  • Opened new possibilities for understanding and optimizing industrial catalytic processes.