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GGA+U method from first principles: application to reduction–oxidation properties in ceria-based oxides

Amra Peles
Journal of Materials Science, 47(21), 7542–7548 (2012)

We implement DFT calculations by a Hubbard-like correction for localized strongly correlated electrons, coupled with a generalized gradient approximation to the exchange-correlation functional to elucidate the role of the ceria based catalytically active supports for the chemical reactions involving reduction–oxidation processes. These catalytic processes are relevant for many industrial applications, such as catalytic converters in automotive applications, solid oxide fuel cells, and hydrogen production from biomass. The Hubbard-like correction U is computed from first principles as physical property of the system. We find that the high performance of ceria-based oxides as an active support for noble metals in catalysis relies on an efficient supply of lattice oxygen at reaction sites governed by oxygen vacancy formation.