Water inhibits CO oxidation on gold cations in the gas phase. Structures and binding energies of the sequential addition of CO, H2O, O2, and N2 onto Au+
| Autor: | Khaled Saoud, M. Samy El-Shall, J. Ulises Reveles |
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| Rok vydání: | 2016 |
| Předmět: |
Addition reaction
Chemistry Inorganic chemistry Binding energy Strong interaction General Physics and Astronomy 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Nanomaterial-based catalyst 0104 chemical sciences Impurity Physical chemistry Molecule Physical and Theoretical Chemistry 0210 nano-technology Saturation (chemistry) Stoichiometry |
| Zdroj: | Physical Chemistry Chemical Physics. 18:28606-28616 |
| ISSN: | 1463-9084 1463-9076 |
| Popis: | We report a detailed experimental and theoretical study of the gas phase reactivity of Au+ with CO, O2, N2 and their mixtures in the presence of a trace amount of water impurity. The gold cation is found to strongly interact with CO and H2O molecules via successive addition reactions until reaching saturation. The stoichiometry of the formed complex is determined by the strength of the binding energy of the neutral molecule to the gold cation. CO binds the strongest to Au+, followed by H2O, N2 and then O2. We found that the gold cation (Au+) can activate the O2 molecule within the Au+(CO)2(O2) complex which could react with another CO molecule to form Au+(CO)(CO2) + CO2. The product Au+(CO)(CO2) is observed experimentally with a small intensity at room temperature. However, the presence of water leads to the formation of Au+(CO)(H2O)(O2) instead of Au+(CO)2(O2) due to the strong interaction between Au+ and water. The current experiments and calculations might lead to a molecular level understanding of the interactions between the active sites, reactants and impurities which could pave the way for the design of efficient nanocatalysts. |
| Databáze: | OpenAIRE |
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