Conversion of methane to benzene in CVI by density functional theory study
| Autor: | Ningning Yan, Tiyuan Wang, Qiang Song, Kun Li, Wei Li, Hejun Li |
|---|---|
| Jazyk: | angličtina |
| Rok vydání: | 2019 |
| Předmět: |
Materials science
Reaction mechanisms Thermodynamics lcsh:Medicine 02 engineering and technology 010402 general chemistry 01 natural sciences Dissociation (chemistry) Article symbols.namesake Transition state theory Reaction rate constant lcsh:Science Basis set Arrhenius equation Multidisciplinary lcsh:R 021001 nanoscience & nanotechnology Transition state 0104 chemical sciences Chemical vapor infiltration symbols Density functional theory Atomistic models lcsh:Q 0210 nano-technology Quantum chemistry |
| Zdroj: | Scientific Reports, Vol 9, Iss 1, Pp 1-11 (2019) Scientific Reports |
| ISSN: | 2045-2322 |
| DOI: | 10.1038/s41598-019-56136-0 |
| Popis: | A density functional theory (DFT) study was employed to explore the mechanism of the conversion of methane to benzene in chemical vapor infiltration (CVI) based on the concluded reaction pathways from C1-species to C6-species. The geometry optimization and vibrational frequency analysis of all the chemical species and transition states (TS) were performed with B3LYP along with a basis set of 6–311 +G(d, p), and Gaussian 09 software was used to perform the study. The rate constants were calculated by KiSThelP according to the conventional transition state theory (TST), and the Wigner method was applied to acquire the tunneling correction factors. Then the rate constants were fitted to the modified Arrhenius expression in the temperature range of 800–2000 K. As for the barrierless reactions calculated in this paper, the rate constants were selected from the relating references. Through the energetic and kinetic calculations, the most favorable reaction pathway for benzene formation from methane was determined, which were mainly made of the unimolecular dissociation. The conversion trend from C1-species to C4-species is mainly guided by a strong tendency to dehydrogenation and the pathways from C4-species to C6-species are all presumed to be able to produce C6H6 molecule. |
| Databáze: | OpenAIRE |
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