Mechanism of methane formation during toluene pyrolysis using DFT calculation
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Mechanism of methane formation during toluene pyrolysis using DFT calculation
CIESC JournalIssue 12, Pages: 3235-3242(2010)
作者机构:
1. 太原理工大学煤科学与技术教育部和山西省重点实验室,地球科学与工程系,山西,太原,030024
2. 河南理工大学材料学院,河南,焦作,454000
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Online First:05 December 2010,
Published:05 December 2010
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JIA Jianbo, ZENG Fangui, LI Meifen, et al. Mechanism of methane formation during toluene pyrolysis using DFT calculation[J]. CIESC Journal, 2010, (12): 3235-3242.
DOI:
JIA Jianbo, ZENG Fangui, LI Meifen, et al. Mechanism of methane formation during toluene pyrolysis using DFT calculation[J]. CIESC Journal, 2010, (12): 3235-3242.DOI:
Mechanism of methane formation during toluene pyrolysis using DFT calculation
The greater part of macromolecule aromatic structure unit of low-rank coal contains mainly 1—2 rings. In order to understand the mechanism of methane formation during coal pyrolysis
the thermodynamics and kinetics calculation were conducted for toluene pyrolysis using DFT method. The results showed that the rate-control step is the dehydrogenization or demethylation process for all routes of methane formation. The energy barrier of toluene demethylation can be significantly reduced by the participation of hydrogen free radical. When temperature is lower than 675 K
the formation of methane is mainly through the following steps: firstly
breaking of the C—H bond in methyl of toluene; secondly
the hydrogen free radical formed adds to the toluene in ipso position and then demethylation; finally
formation of methane is from the formed methyl that captures a hydrogen atom in side chain of toluene. When temperature is higher than 975 K
methane is mainly from toluene demethylation first and then the formed methyl captures a hydrogen atom in side chain of toluene. When the temperature is between 675 K and 975 K
formation of methane is a competitive result of the two routes mentioned above.