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Surface Functionalization of Metal-Organic Frameworks for Improved Moisture Resistance

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Published on: September 5, 2018

CO oxidation on PdO surfaces.

Janne T Hirvi¹, Toni-Jani J Kinnunen, Mika Suvanto

¹Department of Chemistry, University of Eastern Finland, P.O. Box 111, FI-80101 Joensuu, Finland. janne.hirvi@uef.fi

The Journal of Chemical Physics

|September 7, 2010

Summary

Density functional calculations reveal palladium oxide (PdO) surfaces exhibit varied CO oxidation activity. The PdO(100)-O surface shows high activity via the Eley-Rideal mechanism, aligning with experimental data.

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Area of Science:

Surface Science
Computational Chemistry
Catalysis

Background:

Palladium oxide (PdO) is a crucial material in catalytic oxidation reactions.
Understanding CO oxidation mechanisms on PdO surfaces is vital for catalyst design.
Previous studies have explored CO oxidation on metallic palladium but less on PdO.

Purpose of the Study:

To investigate the mechanisms and energetics of CO oxidation on the most stable bulk PdO surfaces.
To compare the reactivity of different PdO surface facets (PdO(100) and PdO(101)).
To elucidate the role of surface oxygen species and reaction pathways.

Main Methods:

Density functional theory (DFT) calculations were employed.
Investigated CO adsorption and oxidation on PdO(100) and PdO(101) surfaces.
Analyzed reaction pathways including Langmuir-Hinshelwood and Eley-Rideal mechanisms.

Main Results:

The stoichiometric PdO(101) surface facilitates CO oxidation via Langmuir-Hinshelwood with an activation energy of 0.66 eV.
The oxygen-rich PdO(100)-O surface exhibits highly favorable CO oxidation through the Eley-Rideal mechanism (0.24 eV activation energy).
Surface oxygen coverage and site blocking influence reaction rates and the potential formation of carbonate species.

Conclusions:

The PdO(100)-O surface demonstrates significant catalytic activity for CO oxidation, particularly via the Eley-Rideal pathway.
The calculated activation energy for palladium-activated CO oxidation on PdO(100)-O agrees well with experimental observations.
Surface structure and oxygen stoichiometry critically determine the CO oxidation mechanism and efficiency on PdO.