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Structure–deactivation relationships in zeolites during the methanol–to-hydrocarbons reaction: Complementary assessments of the coke content.

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Title: Structure–deactivation relationships in zeolites during the methanol–to-hydrocarbons reaction: Complementary assessments of the coke content.
Authors: Rojo-Gama, Daniel1, Signorile, Matteo2, Bonino, Francesca2, Bordiga, Silvia2, Olsbye, Unni1, Lillerud, Karl Petter1, Beato, Pablo3 pabb@topsoe.dk, Svelle, Stian1 stian.svelle@kjemi.uio.no
Source: Journal of Catalysis. Jul2017, Vol. 351, p33-48. 16p.
Subjects: Zeolites, Methanol, Hydrocarbons, Mordenite, Catalysts
Abstract: Catalyst deactivation during the methanol-to-hydrocarbons (MTH) reaction was investigated using five different commercially prepared microporous catalysts, including Mordenite, ZSM-22, ZSM-5, zeolite Beta and SAPO-34. The reaction was carried out in a fixed bed reactor at a constant feed rate per gram of catalyst. Deactivated and partially deactivated catalysts were obtained at increasing reaction times. The whole of the catalyst beds was characterized using nitrogen adsorption, thermogravimetric analysis, a dissolution-extraction protocol, and UV-Raman spectroscopy, focusing primarily on methods suitable for the quantification of the coke. The results illustrate that topology is the dominant parameter that influences not only catalyst lifetime and product distribution, but also the nature of the species causing the deactivation. For all catalyst topologies, when the entire catalyst bed is examined together, the micropore volume and BET surface area decrease more rapidly than total coke from TGA increases at short reaction times. In the materials with the more restricted access to the internal voids, such as ZSM-22 and SAPO-34, the loss of activity is to a large extent due to species which are soluble in dichloromethane and give rise to distinct features in the Raman spectra. For the Mordenite and Beta catalysts, which have larger pores comprising three dimensional networks, and to some extent for the ZSM-5 catalyst employed, the accumulation of more coke species which are insoluble in dichloromethane, presumably on the external surface of the zeolite crystals, is observed. This is linked to the appearance of more pronounced D and G bands in the Raman spectra, indicative of extended carbon species. [ABSTRACT FROM AUTHOR]
Copyright of Journal of Catalysis is the property of Academic Press Inc. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Data: Structure–deactivation relationships in zeolites during the methanol–to-hydrocarbons reaction: Complementary assessments of the coke content.
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  Data: <searchLink fieldCode="JN" term="%22Journal+of+Catalysis%22">Journal of Catalysis</searchLink>. Jul2017, Vol. 351, p33-48. 16p.
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  Data: <searchLink fieldCode="DE" term="%22Zeolites%22">Zeolites</searchLink><br /><searchLink fieldCode="DE" term="%22Methanol%22">Methanol</searchLink><br /><searchLink fieldCode="DE" term="%22Hydrocarbons%22">Hydrocarbons</searchLink><br /><searchLink fieldCode="DE" term="%22Mordenite%22">Mordenite</searchLink><br /><searchLink fieldCode="DE" term="%22Catalysts%22">Catalysts</searchLink>
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  Data: Catalyst deactivation during the methanol-to-hydrocarbons (MTH) reaction was investigated using five different commercially prepared microporous catalysts, including Mordenite, ZSM-22, ZSM-5, zeolite Beta and SAPO-34. The reaction was carried out in a fixed bed reactor at a constant feed rate per gram of catalyst. Deactivated and partially deactivated catalysts were obtained at increasing reaction times. The whole of the catalyst beds was characterized using nitrogen adsorption, thermogravimetric analysis, a dissolution-extraction protocol, and UV-Raman spectroscopy, focusing primarily on methods suitable for the quantification of the coke. The results illustrate that topology is the dominant parameter that influences not only catalyst lifetime and product distribution, but also the nature of the species causing the deactivation. For all catalyst topologies, when the entire catalyst bed is examined together, the micropore volume and BET surface area decrease more rapidly than total coke from TGA increases at short reaction times. In the materials with the more restricted access to the internal voids, such as ZSM-22 and SAPO-34, the loss of activity is to a large extent due to species which are soluble in dichloromethane and give rise to distinct features in the Raman spectra. For the Mordenite and Beta catalysts, which have larger pores comprising three dimensional networks, and to some extent for the ZSM-5 catalyst employed, the accumulation of more coke species which are insoluble in dichloromethane, presumably on the external surface of the zeolite crystals, is observed. This is linked to the appearance of more pronounced D and G bands in the Raman spectra, indicative of extended carbon species. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Journal of Catalysis is the property of Academic Press Inc. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.1016/j.jcat.2017.04.015
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      – Code: eng
        Text: English
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        PageCount: 16
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      – SubjectFull: Zeolites
        Type: general
      – SubjectFull: Methanol
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      – SubjectFull: Hydrocarbons
        Type: general
      – SubjectFull: Mordenite
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      – SubjectFull: Catalysts
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      – TitleFull: Structure–deactivation relationships in zeolites during the methanol–to-hydrocarbons reaction: Complementary assessments of the coke content.
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              Text: Jul2017
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