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Suppression of the aromatic cycle in methanol-to-olefins reaction over ZSM-5 by post-synthetic modification using calcium

(2016) ChemCatChem. 8(19). p.3057-3063
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Abstract
Incorporation of Ca in ZSM-5 results in a twofold increase of propylene selectivity (53%), a total light-olefin selectivity of 90%, and a nine times longer catalyst lifetime (throughput 792 g(MeOH)g(catalyst)(-1)) in the methanol-to-olefins (MTO) reaction. Analysis of the product distribution and theoretical calculations reveal that post-synthetic modification with Ca2+ leads to the formation of CaOCaOH+ that strongly weaken the acid strength of the zeolite. As a result, the rate of hydride transfer and oligomerization reactions on these sites is greatly reduced, resulting in the suppression of the aromatic cycle. Our results further highlight the importance of acid strength on product selectivity and zeolite lifetime in MTO chemistry.
Keywords
Physical and Theoretical Chemistry, Inorganic Chemistry, Organic Chemistry, Catalysis, SOLID-STATE NMR, DENSITY-FUNCTIONAL THEORY, HIGH-SILICA HZSM-5, CATALYTIC PERFORMANCE, SELECTIVE OXIDATION, SHAPE SELECTIVITY, ZEOLITE H-ZSM-5, ACID PROPERTIES, DIMETHYL ETHER, ACTIVE-SITES

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Citation

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Chicago
Yarulina, Irina, Simon Bailleul, Alexey Pustovarenko, Javier Ruiz Martinez, Kristof De Wispelaere, Julianna Hajek, Bert M. Weckhuysen, et al. 2016. “Suppression of the Aromatic Cycle in Methanol-to-olefins Reaction over ZSM-5 by Post-synthetic Modification Using Calcium.” ChemCatChem 8 (19): 3057–3063.
APA
Yarulina, I., Bailleul, S., Pustovarenko, A., Martinez, J. R., De Wispelaere, K., Hajek, J., Weckhuysen, B. M., et al. (2016). Suppression of the aromatic cycle in methanol-to-olefins reaction over ZSM-5 by post-synthetic modification using calcium. ChemCatChem, 8(19), 3057–3063.
Vancouver
1.
Yarulina I, Bailleul S, Pustovarenko A, Martinez JR, De Wispelaere K, Hajek J, et al. Suppression of the aromatic cycle in methanol-to-olefins reaction over ZSM-5 by post-synthetic modification using calcium. ChemCatChem. Wiley-Blackwell; 2016;8(19):3057–63.
MLA
Yarulina, Irina, Simon Bailleul, Alexey Pustovarenko, et al. “Suppression of the Aromatic Cycle in Methanol-to-olefins Reaction over ZSM-5 by Post-synthetic Modification Using Calcium.” ChemCatChem 8.19 (2016): 3057–3063. Print.
@article{8501529,
  abstract     = {Incorporation of Ca in ZSM-5 results in a twofold increase of propylene selectivity (53\%), a total light-olefin selectivity of 90\%, and a nine times longer catalyst lifetime (throughput 792 g(MeOH)g(catalyst)(-1)) in the methanol-to-olefins (MTO) reaction. Analysis of the product distribution and theoretical calculations reveal that post-synthetic modification with Ca2+ leads to the formation of CaOCaOH+ that strongly weaken the acid strength of the zeolite. As a result, the rate of hydride transfer and oligomerization reactions on these sites is greatly reduced, resulting in the suppression of the aromatic cycle. Our results further highlight the importance of acid strength on product selectivity and zeolite lifetime in MTO chemistry.},
  author       = {Yarulina, Irina and Bailleul, Simon and Pustovarenko, Alexey and Martinez, Javier Ruiz and De Wispelaere, Kristof and Hajek, Julianna and Weckhuysen, Bert M. and Houben, Klaartje and Baldus, Marc and Van Speybroeck, Veronique and Kapteijn, Freek and Gascon, Jorge},
  issn         = {1867-3880},
  journal      = {ChemCatChem},
  keyword      = {Physical and Theoretical Chemistry,Inorganic Chemistry,Organic Chemistry,Catalysis,SOLID-STATE NMR,DENSITY-FUNCTIONAL THEORY,HIGH-SILICA HZSM-5,CATALYTIC PERFORMANCE,SELECTIVE OXIDATION,SHAPE SELECTIVITY,ZEOLITE H-ZSM-5,ACID PROPERTIES,DIMETHYL ETHER,ACTIVE-SITES},
  language     = {eng},
  number       = {19},
  pages        = {3057--3063},
  publisher    = {Wiley-Blackwell},
  title        = {Suppression of the aromatic cycle in methanol-to-olefins reaction over ZSM-5 by post-synthetic modification using calcium},
  url          = {http://dx.doi.org/10.1002/cctc.201600650},
  volume       = {8},
  year         = {2016},
}

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