We studied decomposition pathways of ethanol on Ru(0001) with periodic slab-model calculations using a DFT-GGA approach. We calculated the adsorption modes of ethanol and several of its dehydrogenation products and we evaluated reaction energies as well as activation barriers of pertinent dehydrogenation, C-C, and C-O cleavage steps. The calculated barrier heights of C-C and C-O scission steps can be related to the number of hydrogen atoms bound to the C1-C2 and C1-O moieties of the intermediates, respectively. Two counteracting effects are at work, increasing with each dehydrogenation: (i) higher order of the pertinent bond of the adsorbate, and (ii) stronger substrate-surface interaction and thus better stabilization of the transition state. For most intermediates we determined C-O cleavage to be both kinetically and thermodynamically favored over C-C scission, except for the highly dehydrogenated species CH (k) CO (     «

We studied decomposition pathways of ethanol on Ru(0001) with periodic slab-model calculations using a DFT-GGA approach. We calculated the adsorption modes of ethanol and several of its dehydrogenation products and we evaluated reaction energies as well as activation barriers of pertinent dehydrogenation, C-C, and C-O cleavage steps. The calculated barrier heights of C-C and C-O scission steps can be related to the number of hydrogen atoms bound to the C1-C2 and C1-O moieties of the intermediate...     »

ISI Document Delivery No.: 181JP Times Cited: 0 Cited Reference Count: 60 Chiu, Cheng-chau Genest, Alexander Roesch, Notker Fonds der Chemischen Industrie; International Graduate School of Science and Engineering at Technische Universitat Munchen C.C.C. is grateful for a fellowship by the International Graduate School of Science and Engineering at Technische Universitat Munchen. The work of N.R. was supported by Fonds der Chemischen Industrie. We acknowledge generous computing resources at Leibniz Rechenzentrum Munchen. 0 Springer/plenum publishers New york     «

ISI Document Delivery No.: 181JP Times Cited: 0 Cited Reference Count: 60 Chiu, Cheng-chau Genest, Alexander Roesch, Notker Fonds der Chemischen Industrie; International Graduate School of Science and Engineering at Technische Universitat Munchen C.C.C. is grateful for a fellowship by the International Graduate School of Science and Engineering at Technische Universitat Munchen. The work of N.R. was supported by Fonds der Chemischen Industrie. We acknowledge generous computing resources at Leib...     »