PNNL

Abstract

Understanding the dynamics of surface-bound intermediates can provide critical insight into the design and control of catalytically active surfaces for efficient chemical transformation. In particular, titania has drawn significant attention as a model system to provide general insight into the chemistry of oxide surfaces.1–4 Titania is a versatile reducible oxide that is used in numerous catalytic applications, including water splitting,5–7 alcohol oxidation,8,9 CO2 reduction,10–12 and ketonization.13–16 While rutile is the lowest energy polymorph of titania, anatase is more stable in a nanoparticulate form due to the lower surface energies. Both polymorphs and their interfaces are also of significant interest in photocatalysis This work was supported by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program, FWP 47319. PNNL is a multiprogram national laboratory operated for DOE by Battelle under Contract DE-AC05-76RL01830. Computational resources were provided by a user proposal at the National Energy Research Scientific Computing Center located at Lawrence Berkley National Laboratory.