Reaction of CO2 with UO3 Nanoclusters
| Autor: | Luis A. Flores, David A. Dixon, William B. Copeland, Julia G. Murphy |
|---|---|
| Rok vydání: | 2017 |
| Předmět: |
Chemistry
Dimer Trimer 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology Uranyl 01 natural sciences 0104 chemical sciences Nanoclusters Crystallography chemistry.chemical_compound Adsorption Physisorption Chemisorption Computational chemistry Density functional theory Physical and Theoretical Chemistry 0210 nano-technology |
| Zdroj: | The Journal of Physical Chemistry A. 121:8518-8524 |
| ISSN: | 1520-5215 1089-5639 |
| DOI: | 10.1021/acs.jpca.7b09107 |
| Popis: | Adsorption of CO2 to uranium oxide, (UO3)n, clusters was modeled using density functional theory (DFT) and coupled cluster theory (CCSD(T)). Geometries and reaction energies were predicted for carbonate formation (chemisorption) and Lewis acid–base addition of CO2 (physisorption) to these (UO3)n clusters. Chemisorption of multiple CO2 moieties was also modeled for dimer and trimer clusters. Physisorption and chemisorption were both predicted to be thermodynamically allowed for (UO3)n clusters, with chemisorption being more thermodynamically favorable than physisorption. The most energetically favored (UO3)3(CO2)m clusters contain tridentate carbonates, which is consistent with solid-state and solution structures for uranyl carbonates. The calculations show that CO2 exposure is likely to convert (UO3)n to uranyl carbonates. |
| Databáze: | OpenAIRE |
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