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Ag-Cu catalysts for ethylene epoxidation: Selectivity and activity descriptors
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The ultrasolft pseudopotentials for Ag, Cu, O, C, and H were taken from QUANTUM-ESPRESSO pseudopotential download page, see http://www.quantum-espresso.org
(files: Ag.pbe-d-rrkjus.UPF, Cu.pbe-d-rrkjus.UPF, O.pbe-rrkjus.UPF, C.pbe-rrkjus.UPF, and H.pbe-rrkjus.UPF).
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Ag-Cu alloy catalysts for ethylene epoxidation have been shown to yield higher selectivity towards ethylene oxide compared to pure Ag, the unique catalyst employed in the industrial process. Previous studies showed that under oxidizing conditions Cu forms oxide layers on top of Ag. Using first-principles atomistic simulations based on density functional theory, we investigate the reaction mechanism on the thin oxide layer structures and establish the reasons for the improved selectivity. We extend the range of applicability of the selectivity descriptor proposed by Kokalj et al. [J. Catal.254, 304 (Year: 2008)]10.1016/j.jcat.2008.01.008, based on binding energies of reactants, intermediates, and products, by refitting its parameters so as to include thin oxide layer catalysts. We show that the selectivity is mainly controlled by the relative strength of the metal-carbon vs. metal-oxygen bonds, while the height of the reaction barriers mostly depend on the binding energy of the common oxametallacycle intermediate.
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