Journal
ACS CATALYSIS
Volume 5, Issue 1, Pages 317-326Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cs5015749
Keywords
methanol-to-olefin conversion; H-SAPO-34; dual cycle mechanism; polymethylcyclopentenyl cations; polymethylcyclohexenyl cations; density functional theory calculation
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Funding
- National Natural Science Foundation of China [21303089, 21103231, 21421001]
- Municipal Natural Science Foundation of Tianjin [14JCQNJC05700]
- China Postdoctoral Science Foundation [2013M530870, 2014T70211]
- 111 Project [B12015]
- Ministry of Education of China [IRT13R30, IRT13022]
- Deutsche Forschungsgemeinschaft
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Little is known on the early stages of the methanol-to-olefin (MTO) conversion over H-SAPO-34, before the steady-state with highly active polymethylbenzenium cations as most important intermediates is reached. In this work, the formation and evolution of carbenium ions during the early stages of the MTO conversion on a H-SAPO-34 model catalyst were clarified via H-1 MAS NMR and C-13 MAS NMR. Several initial species (i.e., three-ring compounds, dienes, polymethylcyclopentenyl, and polymethylcyclohexenyl cations) were, for the first time, directly verified during the MTO conversion. Their detailed evolution network was established from theoretical calculations. On the basis of these results, an olefm-based catalytic cycle is proposed to be the primary reaction pathway during the early stages of the MTO reaction over H-SAPO-34. After that, an aromatic-based cycle may be involved in the MTO conversion for long times on stream.
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