Cargando…
Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation
Small pore zeolites have shown great potential in a number of catalytic reactions. While Mo-containing medium pore zeolites have been widely studied for methane dehydroaromatisation (MDA), the use of small pore supports has drawn limited attention due to the fast deactivation of the catalyst. This w...
Autores principales: | , , , , , , , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
MDPI
2020
|
Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7663607/ https://www.ncbi.nlm.nih.gov/pubmed/33143211 http://dx.doi.org/10.3390/molecules25215048 |
_version_ | 1783609666345893888 |
---|---|
author | Agote-Arán, Miren Kroner, Anna B. Wragg, David S. Sławiński, Wojciech A. Briceno, Martha Islam, Husn U. Sazanovich, Igor V. Rivas, María E. Smith, Andrew W. J. Collier, Paul Lezcano-González, Inés Beale, Andrew M. |
author_facet | Agote-Arán, Miren Kroner, Anna B. Wragg, David S. Sławiński, Wojciech A. Briceno, Martha Islam, Husn U. Sazanovich, Igor V. Rivas, María E. Smith, Andrew W. J. Collier, Paul Lezcano-González, Inés Beale, Andrew M. |
author_sort | Agote-Arán, Miren |
collection | PubMed |
description | Small pore zeolites have shown great potential in a number of catalytic reactions. While Mo-containing medium pore zeolites have been widely studied for methane dehydroaromatisation (MDA), the use of small pore supports has drawn limited attention due to the fast deactivation of the catalyst. This work investigates the structure of the small pore Mo/H-SSZ-13 during catalyst preparation and reaction by operando X-ray absorption spectroscopy (XAS), in situ synchrotron powder diffraction (SPD), and electron microscopy; then, the results are compared with the medium pore Mo/H-ZSM-5. While SPD suggests that during catalyst preparation, part of the MoO(x) anchors inside the pores, Mo dispersion and subsequent ion exchange was less effective in the small pore catalyst, resulting in the formation of mesopores and Al(2)(M(O)O(4))(3) particles. Unlike Mo/H-ZSM-5, part of the Mo species in Mo/H-SSZ-13 undergoes full reduction to Mo(0) during MDA, whereas characterisation of the spent catalyst indicates that differences also exist in the nature of the formed carbon deposits. Hence, the different Mo speciation and the low performance on small pore zeolites can be attributed to mesopores formation during calcination and the ineffective ion exchange into well dispersed Mo-oxo sites. The results open the scope for the optimisation of synthetic routes to explore the potential of small pore topologies. |
format | Online Article Text |
id | pubmed-7663607 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | MDPI |
record_format | MEDLINE/PubMed |
spelling | pubmed-76636072020-11-14 Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation Agote-Arán, Miren Kroner, Anna B. Wragg, David S. Sławiński, Wojciech A. Briceno, Martha Islam, Husn U. Sazanovich, Igor V. Rivas, María E. Smith, Andrew W. J. Collier, Paul Lezcano-González, Inés Beale, Andrew M. Molecules Article Small pore zeolites have shown great potential in a number of catalytic reactions. While Mo-containing medium pore zeolites have been widely studied for methane dehydroaromatisation (MDA), the use of small pore supports has drawn limited attention due to the fast deactivation of the catalyst. This work investigates the structure of the small pore Mo/H-SSZ-13 during catalyst preparation and reaction by operando X-ray absorption spectroscopy (XAS), in situ synchrotron powder diffraction (SPD), and electron microscopy; then, the results are compared with the medium pore Mo/H-ZSM-5. While SPD suggests that during catalyst preparation, part of the MoO(x) anchors inside the pores, Mo dispersion and subsequent ion exchange was less effective in the small pore catalyst, resulting in the formation of mesopores and Al(2)(M(O)O(4))(3) particles. Unlike Mo/H-ZSM-5, part of the Mo species in Mo/H-SSZ-13 undergoes full reduction to Mo(0) during MDA, whereas characterisation of the spent catalyst indicates that differences also exist in the nature of the formed carbon deposits. Hence, the different Mo speciation and the low performance on small pore zeolites can be attributed to mesopores formation during calcination and the ineffective ion exchange into well dispersed Mo-oxo sites. The results open the scope for the optimisation of synthetic routes to explore the potential of small pore topologies. MDPI 2020-10-30 /pmc/articles/PMC7663607/ /pubmed/33143211 http://dx.doi.org/10.3390/molecules25215048 Text en © 2020 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Article Agote-Arán, Miren Kroner, Anna B. Wragg, David S. Sławiński, Wojciech A. Briceno, Martha Islam, Husn U. Sazanovich, Igor V. Rivas, María E. Smith, Andrew W. J. Collier, Paul Lezcano-González, Inés Beale, Andrew M. Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation |
title | Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation |
title_full | Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation |
title_fullStr | Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation |
title_full_unstemmed | Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation |
title_short | Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation |
title_sort | understanding the deactivation phenomena of small-pore mo/h-ssz-13 during methane dehydroaromatisation |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7663607/ https://www.ncbi.nlm.nih.gov/pubmed/33143211 http://dx.doi.org/10.3390/molecules25215048 |
work_keys_str_mv | AT agotearanmiren understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT kronerannab understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT wraggdavids understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT sławinskiwojciecha understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT bricenomartha understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT islamhusnu understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT sazanovichigorv understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT rivasmariae understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT smithandrewwj understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT collierpaul understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT lezcanogonzalezines understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation AT bealeandrewm understandingthedeactivationphenomenaofsmallporemohssz13duringmethanedehydroaromatisation |