Identifying the general trend of activity of non-stoichiometric metal oxide phases for CO oxidation on Pd(111)

Ziyun Wang, P. Hu*

*Corresponding author for this work

Research output: Contribution to journalArticle

Abstract

Oxidation state changes under reaction conditions are very common in heterogeneous catalysis. However, due to the limitation of experiment and computational methods, the relation between oxidation state and catalytic activity is not clear. Herein, we obtain the most stable structures of palladium oxide films with different oxidation states on palladium metal surfaces using density functional theory calculations and a state-of-the-art optimization method, namely the particle swarm optimization. These structures clearly show the process of palladium oxide film formation on metallic surfaces. Using CO oxidation as a model reaction, we find that the activities increase first and then decrease with the increase of oxidation states, peaking at Pd4O3. Our findings offer an understanding of the phase transformation and the activity of non-stoichiometric phases.

Original languageEnglish
Pages (from-to)784-789
Number of pages6
JournalScience China Chemistry
Volume62
Issue number6
Early online date29 May 2019
DOIs
Publication statusPublished - 01 Jun 2019

Fingerprint

Carbon Monoxide
Oxides
Metals
Oxidation
Oxide films
Palladium
Computational methods
Particle swarm optimization (PSO)
Catalysis
Density functional theory
Catalyst activity
Phase transitions
Experiments
palladium oxide

Keywords

  • CO oxidation
  • DFT
  • non-stoichiometric
  • oxide

Cite this

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abstract = "Oxidation state changes under reaction conditions are very common in heterogeneous catalysis. However, due to the limitation of experiment and computational methods, the relation between oxidation state and catalytic activity is not clear. Herein, we obtain the most stable structures of palladium oxide films with different oxidation states on palladium metal surfaces using density functional theory calculations and a state-of-the-art optimization method, namely the particle swarm optimization. These structures clearly show the process of palladium oxide film formation on metallic surfaces. Using CO oxidation as a model reaction, we find that the activities increase first and then decrease with the increase of oxidation states, peaking at Pd4O3. Our findings offer an understanding of the phase transformation and the activity of non-stoichiometric phases.",
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Identifying the general trend of activity of non-stoichiometric metal oxide phases for CO oxidation on Pd(111). / Wang, Ziyun; Hu, P.

In: Science China Chemistry, Vol. 62, No. 6, 01.06.2019, p. 784-789.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Identifying the general trend of activity of non-stoichiometric metal oxide phases for CO oxidation on Pd(111)

AU - Wang, Ziyun

AU - Hu, P.

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AB - Oxidation state changes under reaction conditions are very common in heterogeneous catalysis. However, due to the limitation of experiment and computational methods, the relation between oxidation state and catalytic activity is not clear. Herein, we obtain the most stable structures of palladium oxide films with different oxidation states on palladium metal surfaces using density functional theory calculations and a state-of-the-art optimization method, namely the particle swarm optimization. These structures clearly show the process of palladium oxide film formation on metallic surfaces. Using CO oxidation as a model reaction, we find that the activities increase first and then decrease with the increase of oxidation states, peaking at Pd4O3. Our findings offer an understanding of the phase transformation and the activity of non-stoichiometric phases.

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