Oxygen Defects and Surface Chemistry of Ceria: Quantum Chemical Studies Compared to Experiment

Much effort has been spent to study the role of ceria in well-established industrial processes such as fluid catalytic cracking and processes occurring in three-way automotive catalysts. Prerequisite to the design of ceria-based materials, in general, and catalysts and catalytic processes with improved activity, in particular, is an atomistic understanding of the catalyst structure and of the elementary catalytic steps. Working in reciprocal or momentum space, use is made of highly optimized and efficient fast Fourier transform (FFT) techniques. The basis set quality is controlled by one parameter, the kinetic energy cutoff, but for a given cutoff the number of plane waves depends on the size of the simulation cell. Differently from basis sets of atom-centered functions, there is no basis set superposition error (BSSE) in plane wave calculations.