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Role of intermediates in reaction pathways from ethene to hydrocarbons over H-ZSM-5

(2017) APPLIED CATALYSIS A-GENERAL. 538. p.207-220
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Abstract
Insight in ethene to hydrocarbon transformation over a H-ZSM-5 catalyst was obtained by means of temporal analysis of products (TAP) in the temperature range 598–698K with pulses of higher olefins, dienes, cyclodienes and aromatics. Pulses of propene, 1-butene and 1-hexene allowed to identify the cracking routes from ethene oligomerization products. When pulsing benzene or ethylbenzene, only accumulation of aromatics occurred. In-situ temperature programmed desorption (TPD) experiments after pulsing identified aromatics as long-lived surface species. The role of intermediates was assessed by means of pre-adsorption ofthe differentfeeds before pulsing ethene, in so-called pump-probe experiments. Butene enhanced propene formation, while all other olefins favored butene production via aliphatic surface intermediates. The latter were also intermediates in the conversion of hexadiene to butene and aromatics, while cyclohexadiene was converted to propene and aromatics via aromatic surface intermediates. In contrast to ethylbenzene pulses alone, aromatics alkylation participated towards light olefin production via sidechain/paring mechanisms. Isotope experiments of 13C2H4 over a catalyst coked during continuous flow experiments with 12C only showed scrambling in both propene and butene products, stressing the role of long-lived aromatic surface intermediates.
Keywords
HZSM-5 ZEOLITE CATALYSTS, TOTAL OXIDATION, COKE FORMATION, REACTION-MECHANISM, SYNTHETIC ZEOLITE, ETHANOL, CONVERSION, METHANOL, CRACKING, ZSM-5

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Chicago
Batchu, Rakesh, Vladimir Galvita, Konstantinos Alexopoulos, Kristof Van der Borght, Hilde Poelman, Marie-Françoise Reyniers, and Guy Marin. 2017. “Role of Intermediates in Reaction Pathways from Ethene to Hydrocarbons over H-ZSM-5.” Applied Catalysis A-general 538: 207–220.
APA
Batchu, R., Galvita, V., Alexopoulos, K., Van der Borght, K., Poelman, H., Reyniers, M.-F., & Marin, G. (2017). Role of intermediates in reaction pathways from ethene to hydrocarbons over H-ZSM-5. APPLIED CATALYSIS A-GENERAL, 538, 207–220.
Vancouver
1.
Batchu R, Galvita V, Alexopoulos K, Van der Borght K, Poelman H, Reyniers M-F, et al. Role of intermediates in reaction pathways from ethene to hydrocarbons over H-ZSM-5. APPLIED CATALYSIS A-GENERAL. 2017;538:207–20.
MLA
Batchu, Rakesh, Vladimir Galvita, Konstantinos Alexopoulos, et al. “Role of Intermediates in Reaction Pathways from Ethene to Hydrocarbons over H-ZSM-5.” APPLIED CATALYSIS A-GENERAL 538 (2017): 207–220. Print.
@article{8536556,
  abstract     = {Insight in ethene to hydrocarbon transformation over a H-ZSM-5 catalyst was obtained by means of temporal analysis of products (TAP) in the temperature range 598--698K with pulses of higher olefins, dienes, cyclodienes and aromatics. Pulses of propene, 1-butene and 1-hexene allowed to identify the cracking routes from ethene oligomerization products. When pulsing benzene or ethylbenzene, only accumulation of aromatics occurred. In-situ temperature programmed desorption (TPD) experiments after pulsing identified aromatics as long-lived surface species. The role of intermediates was assessed by means of pre-adsorption ofthe differentfeeds before pulsing ethene, in so-called pump-probe experiments. Butene enhanced propene formation, while all other olefins favored butene production via aliphatic surface intermediates. The latter were also intermediates in the conversion of hexadiene to butene and aromatics, while cyclohexadiene was converted to propene and aromatics via aromatic surface intermediates. In contrast to ethylbenzene pulses alone, aromatics alkylation participated towards light olefin production via sidechain/paring mechanisms. Isotope experiments of 13C2H4 over a catalyst coked during continuous flow experiments with 12C only showed scrambling in both propene and butene products, stressing the role of long-lived aromatic surface intermediates.},
  author       = {Batchu, Rakesh and Galvita, Vladimir and Alexopoulos, Konstantinos and Van der Borght, Kristof and Poelman, Hilde and Reyniers, Marie-Fran\c{c}oise and Marin, Guy},
  issn         = {0926-860X },
  journal      = {APPLIED CATALYSIS A-GENERAL},
  keyword      = {HZSM-5 ZEOLITE CATALYSTS,TOTAL OXIDATION,COKE FORMATION,REACTION-MECHANISM,SYNTHETIC ZEOLITE,ETHANOL,CONVERSION,METHANOL,CRACKING,ZSM-5},
  language     = {eng},
  pages        = {207--220},
  title        = {Role of intermediates in reaction pathways from ethene to hydrocarbons over H-ZSM-5},
  url          = {http://dx.doi.org/10.1016/j.apcata.2017.03.013},
  volume       = {538},
  year         = {2017},
}

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