Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process

Irina Yarulina; Kristof De Wispelaere; Simon Bailleul; Joris Goetze; Mike Radersma; Edy Abou-Hamad; Ina Vollmer; Maarten Goesten; Brahim Mezari; Emiel J. M. Hensen; Juan S. Martínez-Espín; Magnus Morten; Sharon Mitchell; Javier Perez-Ramirez; Unni Olsbye; Bert M. Weckhuysen; Veronique Van Speybroeck; Freek Kapteijn; Jorge Gascon

doi:10.1038/s41557-018-0081-0

Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process

Irina Yarulina, Kristof De Wispelaere, Simon Bailleul, Joris Goetze, Mike Radersma, Edy Abou-Hamad, Ina Vollmer, Maarten Goesten, Brahim Mezari, Emiel J. M. Hensen, Juan S. Martínez-Espín, Magnus Morten, Sharon Mitchell, Javier Perez-Ramirez, Unni Olsbye, Bert M. Weckhuysen, Veronique Van Speybroeck, Freek Kapteijn, Jorge Gascon

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232 Scopus citations

Abstract

The combination of well-defined acid sites, shape-selective properties and outstanding stability places zeolites among the most practically relevant heterogeneous catalysts. The development of structure–performance descriptors for processes that they catalyse has been a matter of intense debate, both in industry and academia, and the direct conversion of methanol to olefins is a prototypical system in which various catalytic functions contribute to the overall performance. Propylene selectivity and resistance to coking are the two most important parameters in developing new methanol-to-olefin catalysts. Here, we present a systematic investigation on the effect of acidity on the performance of the zeolite ‘ZSM-5’ for the production of propylene. Our results demonstrate that the isolation of Brønsted acid sites is key to the selective formation of propylene. Also, the introduction of Lewis acid sites prevents the formation of coke, hence drastically increasing catalyst lifetime.

Original language	English (US)
Pages (from-to)	804-812
Number of pages	9
Journal	Nature Chemistry
Volume	10
Issue number	8
DOIs	https://doi.org/10.1038/s41557-018-0081-0
State	Published - Jun 25 2018

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: This research received funding from the Netherlands Organization for Scientific Research (NWO) in the framework of the TASC Technology Area ‘Syngas, a Switch to Flexible New Feedstock for the Chemical Industry (TA-Syngas). S.B., K.D.W. and V.V.S. acknowledge the Fund for Scientific Research: Flanders (FWO), the Belgian American Educational Foundation, the Research Board of Ghent University (BOF), BELSPO in the frame of IAP/7/05 and funding from the European Union’s Horizon 2020 research and innovation programme (consolidator ERC grant agreement no. 647755—DYNPOR (2015–2020)). The computational resources and services used were provided by Ghent University (Stevin Supercomputer Infrastructure) and the VSC (Flemish Supercomputer Center), funded by the Research Foundation: Flanders (FWO).

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10.1038/s41557-018-0081-0

https://repository.kaust.edu.sa/bitstream/10754/628296/1/Yarulina%20et%20al%20final.pdf

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Yarulina, I., De Wispelaere, K., Bailleul, S., Goetze, J., Radersma, M., Abou-Hamad, E., Vollmer, I., Goesten, M., Mezari, B., Hensen, E. J. M., Martínez-Espín, J. S., Morten, M., Mitchell, S., Perez-Ramirez, J., Olsbye, U., Weckhuysen, B. M., Van Speybroeck, V., Kapteijn, F., & Gascon, J. (2018). Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process. Nature Chemistry, 10(8), 804-812. https://doi.org/10.1038/s41557-018-0081-0

@article{9c04db480b48470aacb515be606d2ace,

title = "Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process",

abstract = "The combination of well-defined acid sites, shape-selective properties and outstanding stability places zeolites among the most practically relevant heterogeneous catalysts. The development of structure–performance descriptors for processes that they catalyse has been a matter of intense debate, both in industry and academia, and the direct conversion of methanol to olefins is a prototypical system in which various catalytic functions contribute to the overall performance. Propylene selectivity and resistance to coking are the two most important parameters in developing new methanol-to-olefin catalysts. Here, we present a systematic investigation on the effect of acidity on the performance of the zeolite {\textquoteleft}ZSM-5{\textquoteright} for the production of propylene. Our results demonstrate that the isolation of Br{\o}nsted acid sites is key to the selective formation of propylene. Also, the introduction of Lewis acid sites prevents the formation of coke, hence drastically increasing catalyst lifetime.",

author = "Irina Yarulina and {De Wispelaere}, Kristof and Simon Bailleul and Joris Goetze and Mike Radersma and Edy Abou-Hamad and Ina Vollmer and Maarten Goesten and Brahim Mezari and Hensen, {Emiel J. M.} and Mart{\'i}nez-Esp{\'i}n, {Juan S.} and Magnus Morten and Sharon Mitchell and Javier Perez-Ramirez and Unni Olsbye and Weckhuysen, {Bert M.} and {Van Speybroeck}, Veronique and Freek Kapteijn and Jorge Gascon",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This research received funding from the Netherlands Organization for Scientific Research (NWO) in the framework of the TASC Technology Area {\textquoteleft}Syngas, a Switch to Flexible New Feedstock for the Chemical Industry (TA-Syngas). S.B., K.D.W. and V.V.S. acknowledge the Fund for Scientific Research: Flanders (FWO), the Belgian American Educational Foundation, the Research Board of Ghent University (BOF), BELSPO in the frame of IAP/7/05 and funding from the European Union{\textquoteright}s Horizon 2020 research and innovation programme (consolidator ERC grant agreement no. 647755—DYNPOR (2015–2020)). The computational resources and services used were provided by Ghent University (Stevin Supercomputer Infrastructure) and the VSC (Flemish Supercomputer Center), funded by the Research Foundation: Flanders (FWO).",

year = "2018",

month = jun,

day = "25",

doi = "10.1038/s41557-018-0081-0",

language = "English (US)",

volume = "10",

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Yarulina, I, De Wispelaere, K, Bailleul, S, Goetze, J, Radersma, M, Abou-Hamad, E, Vollmer, I, Goesten, M, Mezari, B, Hensen, EJM, Martínez-Espín, JS, Morten, M, Mitchell, S, Perez-Ramirez, J, Olsbye, U, Weckhuysen, BM, Van Speybroeck, V, Kapteijn, F & Gascon, J 2018, 'Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process', Nature Chemistry, vol. 10, no. 8, pp. 804-812. https://doi.org/10.1038/s41557-018-0081-0

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T1 - Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process

AU - Yarulina, Irina

AU - De Wispelaere, Kristof

AU - Bailleul, Simon

AU - Goetze, Joris

AU - Radersma, Mike

AU - Abou-Hamad, Edy

AU - Vollmer, Ina

AU - Goesten, Maarten

AU - Mezari, Brahim

AU - Hensen, Emiel J. M.

AU - Martínez-Espín, Juan S.

AU - Morten, Magnus

AU - Mitchell, Sharon

AU - Perez-Ramirez, Javier

AU - Olsbye, Unni

AU - Weckhuysen, Bert M.

AU - Van Speybroeck, Veronique

AU - Kapteijn, Freek

AU - Gascon, Jorge

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This research received funding from the Netherlands Organization for Scientific Research (NWO) in the framework of the TASC Technology Area ‘Syngas, a Switch to Flexible New Feedstock for the Chemical Industry (TA-Syngas). S.B., K.D.W. and V.V.S. acknowledge the Fund for Scientific Research: Flanders (FWO), the Belgian American Educational Foundation, the Research Board of Ghent University (BOF), BELSPO in the frame of IAP/7/05 and funding from the European Union’s Horizon 2020 research and innovation programme (consolidator ERC grant agreement no. 647755—DYNPOR (2015–2020)). The computational resources and services used were provided by Ghent University (Stevin Supercomputer Infrastructure) and the VSC (Flemish Supercomputer Center), funded by the Research Foundation: Flanders (FWO).

PY - 2018/6/25

Y1 - 2018/6/25

N2 - The combination of well-defined acid sites, shape-selective properties and outstanding stability places zeolites among the most practically relevant heterogeneous catalysts. The development of structure–performance descriptors for processes that they catalyse has been a matter of intense debate, both in industry and academia, and the direct conversion of methanol to olefins is a prototypical system in which various catalytic functions contribute to the overall performance. Propylene selectivity and resistance to coking are the two most important parameters in developing new methanol-to-olefin catalysts. Here, we present a systematic investigation on the effect of acidity on the performance of the zeolite ‘ZSM-5’ for the production of propylene. Our results demonstrate that the isolation of Brønsted acid sites is key to the selective formation of propylene. Also, the introduction of Lewis acid sites prevents the formation of coke, hence drastically increasing catalyst lifetime.

AB - The combination of well-defined acid sites, shape-selective properties and outstanding stability places zeolites among the most practically relevant heterogeneous catalysts. The development of structure–performance descriptors for processes that they catalyse has been a matter of intense debate, both in industry and academia, and the direct conversion of methanol to olefins is a prototypical system in which various catalytic functions contribute to the overall performance. Propylene selectivity and resistance to coking are the two most important parameters in developing new methanol-to-olefin catalysts. Here, we present a systematic investigation on the effect of acidity on the performance of the zeolite ‘ZSM-5’ for the production of propylene. Our results demonstrate that the isolation of Brønsted acid sites is key to the selective formation of propylene. Also, the introduction of Lewis acid sites prevents the formation of coke, hence drastically increasing catalyst lifetime.

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DO - 10.1038/s41557-018-0081-0

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VL - 10

SP - 804

EP - 812

JO - Nature Chemistry

JF - Nature Chemistry

IS - 8

ER -

Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process

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