By R. M. Lambert (auth.), Richard M. Lambert, Gianfranco Pacchioni (eds.)
Heterogeneous catalysis presents the spine of the world's chemical and oil industries. The innate complexity of sensible catalytic structures means that precious growth could be attainable by means of investigating key facets of catalysis through experimental reports on idealised version platforms. skinny movies and supported clusters are promising different types of version method that may be used for this goal, seeing that they mimic very important elements of the homes of functional dispersed catalysts. equally, acceptable theoretical experiences of chemisorption and floor response clusters or prolonged slab platforms grants invaluable info at the elements that underlie bonding and catalytic job. This quantity describes such experimental and theoretical methods to the outside chemistry and catalytic behaviour of metals, steel oxides and metal/metal oxide structures.
An creation to the rules and major issues of heterogeneous catalysis is through unique money owed of the applying of recent experimental and theoretical thoughts to basic difficulties. the appliance of complex experimental tools is complemented by way of a whole description of theoretical approaches, together with Hartree-Fock, density practical and comparable innovations. The relative advantages of a few of the ways are thought of and instructions for destiny development are indicated.
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Additional info for Chemisorption and Reactivity on Supported Clusters and Thin Films: Towards an Understanding of Microscopic Processes in Catalysis
Species plays an important role in determining the activity over Pd. -. :::II 250 500 750 Temperature (K) Figure 19. TPD spectra for 'SN2 recombinative desorption after a 500 L exposure to lWO at the indicated substrate temperatures on Pd(lll) and (lOO). Figure 19 compares TPD for the recombination of N. on Pd(111) and Pd(100) after a 500 L exposure to lSNO in a background pressure of 1 x 10-6 Torr at the indicated substrate temperatures. Following this exposure, the samples were cooled in the presence of the uNO background; the background l~O was subsequently pumped away and the TPD experiment was performed.
Application of negative potential supplies Na to the surface of the catalyst film and leads to a large enhancement in total catalytic rate (the figure shows the N2 rate) and significant improvements in N2 selectivity. At relatively low Na loadings the system exhibits strong promotion: rate increases exponentially with catalyst potential, as predicted theoretically. Eventually, overloading with Na leads to poisoning. It is emphasised that this behaviour is fully reversible - the system could be cycled repeatedly and reproducibly between the promoted and poisoned regimes.
Following this exposure, the samples were cooled in the presence of the uNO background; the background l~O was subsequently pumped away and the TPD experiment was performed. On both surfaces, N2 recombinative desorption occurs in two distinct phases, giving rise to a low temperature and a high temperature feature in the TPD spectrum. However, clear differences between the two surfaces are apparent The total combined peak lSN2 area at each substrate exposure temperature is greater on the (lOO) surface, consistent with more facile NO dissociation on the more open face.
Chemisorption and Reactivity on Supported Clusters and Thin Films: Towards an Understanding of Microscopic Processes in Catalysis by R. M. Lambert (auth.), Richard M. Lambert, Gianfranco Pacchioni (eds.)