期刊
CHEMPHYSCHEM
卷 19, 期 4, 页码 496-503出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201701020
关键词
cyclization; density functional calculations; hydride transfer; linear alkenes; zeolite
资金
- National Natural Science Foundation of China [21573270, U1510104, 21603257, 21773281]
- Natural Science Foundation of Shanxi Province of China [2015021003]
- CAS/SAFEA International Partnership Program for Creative Research Teams [2013131001]
- Innovative Talent Program of Shanxi Province [201605D211001]
- Youth Innovation Promotion Association of Chinese Academy of Sciences [2016161]
Although dienes or trienes have been shown to be possible precursors for cyclization, direct cyclization of alkenes or alkoxides has not been systematically studied yet. Thus, the reaction mechanism of cyclization of linear alkenes over H-ITQ-13 was investigated here by density functional theory considering dispersive interactions (DFT-D). The similar free energy of different linear alkoxides of the same carbon number suggests that they can co-exist in the H-ITQ-13 intersection at 673.15K during the methanol to olefins (MTO) process. The formation of linear alkenes by olefins methylation with methoxyl groups (ZOCH(3)), trimethyloxonium ions (TMO+), and methanol are kinetically more favorable than by dimerization of olefins. Linear alkoxides or alkenes prefer direct cyclization to cycloalkanes rather than hydride transfer to diene. This study provides new insight into the alkene cyclization and aromatization mechanisms in MTO process.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据