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Insight into the effect of water on the methanol-to-olefins conversion in H-SAPO-34 from molecular simulations and in situ microspectroscopy

(2016) ACS CATALYSIS. 6(3). p.1991-2002
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Abstract
The role of water in the methanol-to-olefins (MTO) process over H-SAPO-34 has been elucidated by a combined theoretical and experimental approach, encompassing advanced molecular dynamics simulations and in situ microspectroscopy. First-principles calculations at the molecular level point out that water competes with methanol and propene for direct access to the Bronsted acid sites. This results in less efficient activation of these molecules, which are crucial for the formation of the hydrocarbon pool. Furthermore, lower intrinsic methanol reactivity toward methoxide formation has been observed. These observations are in line with a longer induction period observed from in situ UV-vis microspectroscopy experiments. These experiments revealed a slower and more homogeneous discoloration of H-SAPO-34, while in situ confocal fluorescence microscopy confirmed the more homogeneous distribution and larger amount of MTO intermediates when cofeeding water. As such, it is shown that water induces a more efficient use of the H-SAPO-34 catalyst crystals at the microscopic level. The combined experimental theoretical approach gives a profound insight into the role of water in the catalytic process at the molecular and single-particle level.
Keywords
methanol-to-olefins, NITRILE ADSORPTION, zeolites, water, molecular dynamics, metadynamics, UV-vis spectroscopy, confocal fluorescence microscopy, MICROPOROUS MATERIALS, HYDROCARBON FORMATION, THEORETICAL SIMULATIONS, UV/VIS MICROSPECTROSCOPY, COKE FORMATION, MTO REACTION, REACTION-MECHANISM, PRODUCT SELECTIVITY, ACIDIC ZEOLITE CATALYSTS

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Citation

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MLA
De Wispelaere, Kristof et al. “Insight into the Effect of Water on the Methanol-to-olefins Conversion in H-SAPO-34 from Molecular Simulations and in Situ Microspectroscopy.” ACS CATALYSIS 6.3 (2016): 1991–2002. Print.
APA
De Wispelaere, K., Wondergem, C. S., Ensing, B., Hemelsoet, K., Meijer, E. J., Weckhuysen, B. M., Van Speybroeck, V., et al. (2016). Insight into the effect of water on the methanol-to-olefins conversion in H-SAPO-34 from molecular simulations and in situ microspectroscopy. ACS CATALYSIS, 6(3), 1991–2002.
Chicago author-date
De Wispelaere, Kristof, Caterina S Wondergem, Bernd Ensing, Karen Hemelsoet, Evert Jan Meijer, Bert M Weckhuysen, Veronique Van Speybroeck, and Javier Ruiz-Martinez. 2016. “Insight into the Effect of Water on the Methanol-to-olefins Conversion in H-SAPO-34 from Molecular Simulations and in Situ Microspectroscopy.” Acs Catalysis 6 (3): 1991–2002.
Chicago author-date (all authors)
De Wispelaere, Kristof, Caterina S Wondergem, Bernd Ensing, Karen Hemelsoet, Evert Jan Meijer, Bert M Weckhuysen, Veronique Van Speybroeck, and Javier Ruiz-Martinez. 2016. “Insight into the Effect of Water on the Methanol-to-olefins Conversion in H-SAPO-34 from Molecular Simulations and in Situ Microspectroscopy.” Acs Catalysis 6 (3): 1991–2002.
Vancouver
1.
De Wispelaere K, Wondergem CS, Ensing B, Hemelsoet K, Meijer EJ, Weckhuysen BM, et al. Insight into the effect of water on the methanol-to-olefins conversion in H-SAPO-34 from molecular simulations and in situ microspectroscopy. ACS CATALYSIS. 2016;6(3):1991–2002.
IEEE
[1]
K. De Wispelaere et al., “Insight into the effect of water on the methanol-to-olefins conversion in H-SAPO-34 from molecular simulations and in situ microspectroscopy,” ACS CATALYSIS, vol. 6, no. 3, pp. 1991–2002, 2016.
@article{7173168,
  abstract     = {The role of water in the methanol-to-olefins (MTO) process over H-SAPO-34 has been elucidated by a combined theoretical and experimental approach, encompassing advanced molecular dynamics simulations and in situ microspectroscopy. First-principles calculations at the molecular level point out that water competes with methanol and propene for direct access to the Bronsted acid sites. This results in less efficient activation of these molecules, which are crucial for the formation of the hydrocarbon pool. Furthermore, lower intrinsic methanol reactivity toward methoxide formation has been observed. These observations are in line with a longer induction period observed from in situ UV-vis microspectroscopy experiments. These experiments revealed a slower and more homogeneous discoloration of H-SAPO-34, while in situ confocal fluorescence microscopy confirmed the more homogeneous distribution and larger amount of MTO intermediates when cofeeding water. As such, it is shown that water induces a more efficient use of the H-SAPO-34 catalyst crystals at the microscopic level. The combined experimental theoretical approach gives a profound insight into the role of water in the catalytic process at the molecular and single-particle level.},
  author       = {De Wispelaere, Kristof and Wondergem, Caterina S and Ensing, Bernd and Hemelsoet, Karen and Meijer, Evert Jan and Weckhuysen, Bert M and Van Speybroeck, Veronique and Ruiz-Martinez, Javier},
  issn         = {2155-5435},
  journal      = {ACS CATALYSIS},
  keywords     = {methanol-to-olefins,NITRILE ADSORPTION,zeolites,water,molecular dynamics,metadynamics,UV-vis spectroscopy,confocal fluorescence microscopy,MICROPOROUS MATERIALS,HYDROCARBON FORMATION,THEORETICAL SIMULATIONS,UV/VIS MICROSPECTROSCOPY,COKE FORMATION,MTO REACTION,REACTION-MECHANISM,PRODUCT SELECTIVITY,ACIDIC ZEOLITE CATALYSTS},
  language     = {eng},
  number       = {3},
  pages        = {1991--2002},
  title        = {Insight into the effect of water on the methanol-to-olefins conversion in H-SAPO-34 from molecular simulations and in situ microspectroscopy},
  url          = {http://dx.doi.org/10.1021/acscatal.5b02139},
  volume       = {6},
  year         = {2016},
}

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