DeNox Catalysis and the Quantum Size / d Band filling Model Competition

FREDERIK TIELENS; NUÑEZ, JOSÉ L.; COLOMBO, ESTEFANIA; TRANCA, IONUT; PAOLA QUAINO; BAZIN, DOMINIQUE

Lyon

Congreso; 18th ICC International Congress on Catalysis; 2024

International Congress on Catalysis

The rational design of catalysts used in the Denox process relies on a deepunderstanding of the interaction between molecules such NO, O2, N2 and nanometer scalemetallic clusters.1 Following an approach defined and discussed by Boudart “model catalysts:reductionism for understanding”,2 we have considered a model based on experimental datawhich establishes a relationship between the interaction mode of NO (non-dissociative ordissociative adsorption) and the behavior of nanometer scale metallic cluster (sintering ordisruption) in response to this interaction.3,4 Recent density functional theory (DFT) studies onunsupported mono5-7 and supported bimetallic 8 clusters have validated this relationship. Allthese publications indicate that the reactivity of metal clusters for NO is determined by theenergy and type (4d or 5s) of the valence band top, which both depend on the position of theelement in the periodic table. In this presentation, we would like to share a first set of resultsregarding the adsorption of two other molecules, namely N2 and O2, on monometallic M13(See Figure 1) nanoparticles (M = Ag, Au, Co, Cu, Fe, Ir, Mo, Ni, Os, Pd, Pt, Re, Rh, Ru). In thiscontext we will focus on the clusters cohesive energies, as well as on the metallic meltingpoints.