Peer-Reviewed Journal Details
Mandatory Fields
Garcia, Juan C.;Nolan, Michael; Deskins, N. Aaron
2015
January
Journal of Chemical Physics
The nature of interfaces and charge trapping sites in photocatalytic mixed-phase TiO2 from first principles modeling
Published
WOS: 33 ()
Optional Fields
Ab initio calculations Catalysis Catalysts Conduction bands Density functional theory Electron traps Electron-hole recombination Energy gap Interface states Nanoparticles Photochemistry Reaction kinetics theory Reduction (chemical)
142
024708
Mixed phase rutile/anatase catalysts show increased reactivity compared with the pure phases alone. However, the mechanism causing this effect is not fully understood. The electronic properties of the interface and the relative energy of the electron in each phase play a key role in lowering the rate of recombination of electron hole pairs. Using density functional theory and the +U correction, we calculated the bands offsets between the phases taking into account the effect of the interface. Our model included several thousands atoms, and thus is a good representation of an interface between actual nanoparticles. We found rutile to have both higher conduction and valence band offsets than rutile, leading to an accumulation of electrons in the anatase phase accompanied by hole accumulation in the rutile phase. We also probed the electronic structure of our heterostructure and found a gap state caused by electrons localized in undercoordinated Ti atoms which were present within the interfacial region. Interfaces between bulk materials and between exposed surfaces both showed electron trapping at undercoordinated sites. These undercoordinated (typically four) atoms present localized electrons that could enable reduction reactions in the interfacial region, and could explain the increased reactivity of mixed-phase TiO2 photocatalyst materials. (C) 2015 AIP Publishing LLC.
MELVILLE
0021-9606
http://aip.scitation.org/doi/abs/10.1063/1.4905122
10.1063/1.4905122
Grant Details