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          Institute: MPI für Chemische Physik fester Stoffe     Collection: publications 2013     Display Documents

ID: 671336.0, MPI für Chemische Physik fester Stoffe / publications 2013
Methanol synthesis on ZnO(0001).II. Structure, energetics, and vibrational signature of reaction intermediates
Authors:Kiss, J.; Frenzel, J.; Meyer, B.; Marx, D.
Date of Publication (YYYY-MM-DD):2013-07-28
Title of Journal:Journal of Chemical Physics
Issue / Number:4
Start Page:044705-1
End Page:044705-17
Sequence Number of Article:044705
Review Status:not specified
Audience:Not Specified
Abstract / Description:A rigorous characterization of a wealth of molecular species adsorbed at oxygen defects on ZnO(000 (1) over bar) is given. These defects represent the putative active sites in methanol synthesis from CO and H-2. The oxidation state of the ZnO catalyst and thus the preferred charge state and the reactivity of the oxygen vacancies depend on the gas phase temperature and pressure conditions. Considering charge states of oxygen vacancies relevant at the reducing conditions of the industrial process, i.e., F++/H-2, F-0, F-0/H-2, and F--, as well as the F++ center which is abundant at UHV conditions and therefore important to allow for comparison with surface science experiments, we have investigated the structure, energetics, and vibrational frequencies of an exhaustive catalog of reaction intermediates using electronic structure calculations. After having identified the characteristic adsorption modes of CO, formate, formic acid, hydroxymethylene, formyl, formaldehyde, dioxomethylene, hydroxymethyl, hydroxymethoxide, methoxide, as well as methanol itself, the thermodynamic stability of all species with respect to the charge state of the oxygen vacancy and their electronic stabilization is discussed in detail and summarized in an energy level diagram. (C) 2013 AIP Publishing LLC.
External Publication Status:published
Document Type:Article
Communicated by:Ina Werner
Affiliations:MPI für chemische Physik fester Stoffe
Identifiers:ISI:000322949300051 [ID No:1]
ISSN:0021-9606 [ID No:2]
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