Cargando…
Role of Strontium Cations in ZSM-5 Zeolite in the Methanol-to-Hydrocarbons Reaction
[Image: see text] The selectivity of the methanol-to-hydrocarbons (MTH) reaction can be tuned by modifying zeolite catalysts with alkaline earth metals, which typically increase propylene selectivity and catalyst stability. Here we employed Sr(2+) as its higher atomic number in comparison to the zeo...
Autores principales: | , , , , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
|
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10364136/ https://www.ncbi.nlm.nih.gov/pubmed/37439753 http://dx.doi.org/10.1021/acs.jpclett.3c01259 |
_version_ | 1785076788954660864 |
---|---|
author | Liutkova, Anna Drozhzhin, Victor Heinrichs, Jason M. J. J. Jestl, Valentin Evtushkova, Angelina Mezari, Brahim Mayoral, Álvaro Kosinov, Nikolay Hensen, Emiel J. M. |
author_facet | Liutkova, Anna Drozhzhin, Victor Heinrichs, Jason M. J. J. Jestl, Valentin Evtushkova, Angelina Mezari, Brahim Mayoral, Álvaro Kosinov, Nikolay Hensen, Emiel J. M. |
author_sort | Liutkova, Anna |
collection | PubMed |
description | [Image: see text] The selectivity of the methanol-to-hydrocarbons (MTH) reaction can be tuned by modifying zeolite catalysts with alkaline earth metals, which typically increase propylene selectivity and catalyst stability. Here we employed Sr(2+) as its higher atomic number in comparison to the zeolite T atoms facilitates characterization by scanning transmission electron microscopy and operando X-ray absorption spectroscopy. Sr(2+) dispersed in the ZSM-5 micropores coordinates water, methanol, and dimethyl ether during the MTH reaction. Complementary characterization with nuclear magnetic resonance spectroscopy, thermogravimetric analysis combined with mass spectrometry, operando infrared spectroscopy, and X-ray diffraction points to the retention of substantially more adsorbates during the MTH reaction in comparison to Sr-free zeolites. Our findings support the notion that alkaline earth metals modify the porous reaction environment such that the olefin cycle is favored over the aromatic cycle in the MTH, explaining the increased propylene yield and lower deactivation rate. |
format | Online Article Text |
id | pubmed-10364136 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-103641362023-07-25 Role of Strontium Cations in ZSM-5 Zeolite in the Methanol-to-Hydrocarbons Reaction Liutkova, Anna Drozhzhin, Victor Heinrichs, Jason M. J. J. Jestl, Valentin Evtushkova, Angelina Mezari, Brahim Mayoral, Álvaro Kosinov, Nikolay Hensen, Emiel J. M. J Phys Chem Lett [Image: see text] The selectivity of the methanol-to-hydrocarbons (MTH) reaction can be tuned by modifying zeolite catalysts with alkaline earth metals, which typically increase propylene selectivity and catalyst stability. Here we employed Sr(2+) as its higher atomic number in comparison to the zeolite T atoms facilitates characterization by scanning transmission electron microscopy and operando X-ray absorption spectroscopy. Sr(2+) dispersed in the ZSM-5 micropores coordinates water, methanol, and dimethyl ether during the MTH reaction. Complementary characterization with nuclear magnetic resonance spectroscopy, thermogravimetric analysis combined with mass spectrometry, operando infrared spectroscopy, and X-ray diffraction points to the retention of substantially more adsorbates during the MTH reaction in comparison to Sr-free zeolites. Our findings support the notion that alkaline earth metals modify the porous reaction environment such that the olefin cycle is favored over the aromatic cycle in the MTH, explaining the increased propylene yield and lower deactivation rate. American Chemical Society 2023-07-13 /pmc/articles/PMC10364136/ /pubmed/37439753 http://dx.doi.org/10.1021/acs.jpclett.3c01259 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Liutkova, Anna Drozhzhin, Victor Heinrichs, Jason M. J. J. Jestl, Valentin Evtushkova, Angelina Mezari, Brahim Mayoral, Álvaro Kosinov, Nikolay Hensen, Emiel J. M. Role of Strontium Cations in ZSM-5 Zeolite in the Methanol-to-Hydrocarbons Reaction |
title | Role of Strontium
Cations in ZSM-5 Zeolite
in the Methanol-to-Hydrocarbons Reaction |
title_full | Role of Strontium
Cations in ZSM-5 Zeolite
in the Methanol-to-Hydrocarbons Reaction |
title_fullStr | Role of Strontium
Cations in ZSM-5 Zeolite
in the Methanol-to-Hydrocarbons Reaction |
title_full_unstemmed | Role of Strontium
Cations in ZSM-5 Zeolite
in the Methanol-to-Hydrocarbons Reaction |
title_short | Role of Strontium
Cations in ZSM-5 Zeolite
in the Methanol-to-Hydrocarbons Reaction |
title_sort | role of strontium
cations in zsm-5 zeolite
in the methanol-to-hydrocarbons reaction |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10364136/ https://www.ncbi.nlm.nih.gov/pubmed/37439753 http://dx.doi.org/10.1021/acs.jpclett.3c01259 |
work_keys_str_mv | AT liutkovaanna roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction AT drozhzhinvictor roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction AT heinrichsjasonmjj roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction AT jestlvalentin roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction AT evtushkovaangelina roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction AT mezaribrahim roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction AT mayoralalvaro roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction AT kosinovnikolay roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction AT hensenemieljm roleofstrontiumcationsinzsm5zeoliteinthemethanoltohydrocarbonsreaction |