from first principles PP-I-1

KL-2Catalysis from First Principles:Is it Crucial to Account for the Effects of Nanostructuring?Neyman K.M.Institució Catalana de Recerca i Estudis Avancats (ICREA), Barcelona, SpainDepartament de Química Física & IQTCUB, Universitat de Barcelona, Barcelona, Spainkonstantin.neyman@icrea.catDifference in the complexity of single crystal surfaces and “real” catalysts causes a problemknown as material gap in catalysis. This major obstacle hinders the extension of profoundlyunderstood processes on single crystal surfaces to equally good understanding ofheterogeneous catalysis. Indeed, active components of most working catalysts arenanoparticles exposing defects and irregularities that often control the reactivity. Tounderstand the reactivity of such systems, it is crucial to go beyond the still common singlecrystaldescription. For that, model metal catalysts formed of well-characterized supportednanoparticles have been proven experimentally very fruitful [1].Computational strategy to model experimentally studied catalysis-relevant nanoparticles willbe outlined. Applications to metal [2-5], oxide [6, 7] and metal/oxide [8, 9] nanostructureswill be discussed.References:[1] M. Bäumer, H.-J. Freund, Metal deposits on well-ordered oxide films. Progr. Surf. Sci. 61 (1999) 127.[2] F. Viñes, Y. Lykhach, T. Staudt, M. P. A. Lorenz, C. Papp, H.-P. Steinrück, J. Libuda,K. M. Neyman, A. Görling, Methane activation by platinum: Critical role of edge and corner sites ofmetal nanoparticles. Chemistry - Eur. J. 16 (2010) 6530.[3] I. V. Yudanov, A. V. Matveev, K. M. Neyman, N. Rösch, How the C-O bond breaks duringmethanol decomposition on nanocrystallites of palladium catalysts. J. Am. Chem. Soc. 130 (2008)9342.[4] F. Viñes, C. Loschen, F. Illas, K. M. Neyman, Edge sites as a gate for subsurface carbon inpalladium nanoparticles. J. Catal. 266 (2009) 59.[5] K. M. Neyman, S. Schauermann, Hydrogen diffusion into Pd nanoparticles: Pivotal promotion bycarbon. Angew. Chemie Int. Ed. 49 (2010) 4743.[6] A. Migani, G. N. Vayssilov, S. T. Bromley, F. Illas, K. M. Neyman, Greatly facilitated oxygenvacancy formation in ceria nanocrystallites. Chem. Commun. 46 (2010) 5936.[7] A. Migani, K. M. Neyman, S. T. Bromley, Octahedrality versus tetrahedrality in stoichiometricceria nanoparticles. Chem. Commun. 48 (2012) 4199.[8] G. N. Vayssilov, A. Migani, K. Neyman, Density functional modeling of the interactions ofplatinum clusters with CeO 2 nanoparticles of different size. J. Phys. Chem. C 115 (2011) 16081.[9] G. N. Vayssilov, Y. Lykhach, A. Migani, T. Staudt, G. P. Petrova, N. Tsud, T. Skála, A. Bruix,F. Illas, K. C. Prince, V. Matolin, K. M. Neyman, J. Libuda, Support nanostructure boosts oxygentransfer to catalytically active platinum nanoparticles. Nature Materials 10 (2011) 310.17