1 Department of Physics, Technical University of Denmark2 Center for Atomic-scale Materials Design, Center, Technical University of Denmark3 Purdue University4 University of Jyvaskyla5 Stanford University6 Argonne National Laboratory7 Purdue University8 University of Jyvaskyla9 Stanford University10 Argonne National Laboratory
Periodic Density Functional Theory calculations are capable of providing powerful insights into the structural, energetics, and electronic phenomena that underlie heterogeneous catalysis on transition metal nanoparticles. Such calculations are now routinely applied to single crystal metal surfaces and to subnanometer metal clusters. Descriptions of catalysis on truly nanosized structures, however, are generally not as well developed. In this talk, I will illustrate different approaches to analyzing nanocatalytic phenomena with DFT calculations. I will describe case studies from heterogeneous catalysis and electrocatalysis, in which single crystal models are combined with Wulff construction-based ideas to produce descriptions of average nanocatalyst behavior. Then, I will proceed to describe explicitly DFT-based descriptions of catalysis on truly nanosized particles (<~4 nm in diameter), and I will lay out simple criteria which may be used to determine when unsupported nanoparticles may be described by corresponding single crystal calculations.
Abstracts of Papers of the American Chemical Society, 2013, Vol 246