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

  • Ziyun Wang
  • P. HuEmail author


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.

DFT non-stoichiometric oxide CO oxidation 


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The authors gratefully acknowledge UK’s national high performance computing service ARCHER (for which access was obtained via the UKCP consortium) for computing time. This work was supported by the National Natural Science Foundation of China (21333003) and Queens University Belfast for a Ph.D. studentship.

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Copyright information

© Science China Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  1. 1.School of Chemistry and Chemical EngineeringQueen’s University BelfastBelfastUK

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