Reaction Mechanism for Methane-to-Methanol in Cu-SSZ-13: First-Principles Study of the Z2[Cu2O] and Z2[Cu2OH] Motifs
| Autor: | Anders Hellman, Henrik Grönbeck, Unni Engedahl, Adam Arvidsson |
|---|---|
| Rok vydání: | 2020 |
| Předmět: |
Reaction mechanism
lcsh:Chemical technology DFT Catalysis Methane lcsh:Chemistry small-pore zeolite chemistry.chemical_compound Computational chemistry direct conversion lcsh:TP1-1185 Partial oxidation Physical and Theoretical Chemistry Exergonic reaction methane-to-methanol biology Chemistry Active site SSZ-13 micro-kinetic model TheoryofComputation_MATHEMATICALLOGICANDFORMALLANGUAGES lcsh:QD1-999 copper biology.protein chabazite reaction mechanism Methanol |
| Zdroj: | Catalysts, Vol 11, Iss 17, p 17 (2021) Catalysts Volume 11 Issue 1 |
| ISSN: | 2073-4344 |
| DOI: | 10.3390/catal11010017 |
| Popis: | As transportation continues to increase world-wide, there is a need for more efficient utilization of fossil fuel. One possibility is direct conversion of the solution gas bi-product CH4 into an energy-rich, easily usable liquid fuel such as CH3OH. However, new catalytic materials to facilitate the methane-to-methanol reaction are needed. Using density functional calculations, the partial oxidation of methane is investigated over the small-pore copper-exchanged zeolite SSZ-13. The reaction pathway is identified and the energy landscape elucidated over the proposed motifs Z2[Cu2O] and Z2[Cu2OH]. It is shown that the Z2[Cu2O] motif has an exergonic reaction path, provided water is added as a solvent for the desorption step. However, a micro-kinetic model shows that neither Z2[Cu2O] nor Z2[Cu2OH] has any notable activity under the reaction conditions. These findings highlight the importance of the detailed structure of the active site and that the most stable motif is not necessarily the most active. |
| Databáze: | OpenAIRE |
| Externí odkaz: |
|