Issue 39, 2014

The influence of the Hubbard U parameter in simulating the catalytic behaviour of cerium oxide

Abstract

The seemingly unique redox and oxygen storage properties of cerium oxide (ceria) lead to broad practical application. However, the theoretical treatment of ceria can be troublesome due to the localised nature of the f-electrons and the self-interaction error associated with Density Functional Theory (DFT). DFT + U has been a widely used method to correct for these errors when probing specific physical material properties. However, due to the empirical nature of the U correction it is not immediately obvious that correcting certain bulk properties leads to the correct description of catalytic reactivity at surfaces. We propose an approach to choosing the U parameter using adsorption properties that provides a consistent method to simulate catalytic properties of ceria. We go on to show that combining the derived ceria energetics with those of adsorption at metal surfaces, allow us to construct transition metal–oxide pairings to develop a redox screening model for catalysis.

Graphical abstract: The influence of the Hubbard U parameter in simulating the catalytic behaviour of cerium oxide

Article information

Article type
Paper
Submitted
04 Mar 2014
Accepted
14 Apr 2014
First published
17 Apr 2014

Phys. Chem. Chem. Phys., 2014,16, 21032-21038

Author version available

The influence of the Hubbard U parameter in simulating the catalytic behaviour of cerium oxide

L. J. Bennett and G. Jones, Phys. Chem. Chem. Phys., 2014, 16, 21032 DOI: 10.1039/C4CP00928B

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements