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Controlling Heterogeneous Catalysis With Subsurface Oxygen.

Arved C Dorst1,2, Zhikai Jiang3, Maxwell Gillum4

  • 1Institute of Physical Chemistry, University of Göttingen, Göttingen, Germany.

Angewandte Chemie (International Ed. in English)
|February 18, 2026
PubMed
Summary
This summary is machine-generated.

Subsurface oxygen on rhodium surfaces alters carbon monoxide (CO) oxidation. Without it, CO2 desorbs with high energy; with it, CO2 thermalizes, impacting catalytic activity.

Keywords:
CO oxidation on Rh surfacesDFT calculationsion imagingmolecular beam surface scatteringsubsurface oxygen

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Area of Science:

  • Heterogeneous catalysis
  • Surface science
  • Chemical kinetics

Background:

  • Rhodium surfaces are vital in catalysis, particularly for CO oxidation.
  • Surface oxygen species significantly influence rhodium's catalytic reactivity.
  • Subsurface oxygen can form on rhodium, potentially altering reaction pathways.

Purpose of the Study:

  • To investigate the effect of subsurface oxygen on CO oxidation over single-crystal Rh surfaces.
  • To understand how subsurface oxygen modifies the reaction dynamics and product desorption.
  • To elucidate the role of subsurface oxygen in the CO oxidation mechanism on rhodium.

Main Methods:

  • Molecular beam surface scattering experiments.
  • Ion imaging techniques for product analysis.
  • Ultra-high vacuum (UHV) surface science methods.
  • Density Functional Theory (DFT) calculations.

Main Results:

  • CO oxidation on Rh(2x1)-O adlayer without subsurface oxygen yields hyperthermal CO2 desorption, indicating direct energy release from the transition state.
  • The presence of subsurface oxygen leads to thermalized CO2 velocity distributions.
  • DFT calculations reveal a favored chemisorption state forming with subsurface oxygen, transiently trapping CO2 for thermalization.

Conclusions:

  • Subsurface oxygen fundamentally changes the CO oxidation reaction dynamics on rhodium.
  • The formation of a transient chemisorption state by subsurface oxygen leads to product thermalization.
  • Understanding these effects is crucial for designing efficient rhodium-based catalysts.