First-principles based models for lateral interactions of adsorbates [Elektronische Ressource] / vorgelegt von Michael Rieger

Freie Universität BerlinFachbereich PhysikFirst-principles based models forlateral interactions of adsorbatesvorgelegt vonim Fachbereich PhysikMichael Riegerder Freien Universität Berlineingereichte Dissertation zur Erlangung desakademischen GradesBerlin,2010DOCTOR RERUM NATURALIUMiiThisPhDworkwascarriedoutundersupervisionofProf. Dr. KarstenReuterintheTheoryDepartmentofProf. MatthiasSchefflerattheFritz-Haber-InstituteoftheMax-Planck-SocietybetweenMarch2007andAugust2010.Gutachter1. Gutachter/Betreuer: Prof. Dr. KarstenReuter2. Gutachter: Prof. Dr. MartinWolfDateofdefense: 01.11.2010iiiEvertried. Everfailed.Nomatter.Tryagain. Failagain.Failbetter.SamuelBeckett,WorstwardHo-1983«madeonamac»ivAbstractTheadsorptionofaparticleormoleculefromthegas-phaseiswhatistypicallyreferredtoasthe first step in heterogeneously catalyzed processes. The adsorbed particles are activatedforthesubsequentchemicalreactionbythechemicalbondbeingformedbetweentheparticleand the specific adsorption site on the surface. How reactive an adsorbed particle will be isstrongly influenced by the strength of this bond to the surface. A strong bonding to thesurface can lead to a low reactivity. In case of a weak bond, it is possible that the particledesorbsagainbeforeareactioncouldtakeplace.