Improved Dimethyl Ether Production from Syngas over Aerogel Sulfated Zirconia and Cu-ZnO(Al) Bifunctional Composite Catalysts

This work is dedicated to the study of the effect of the synthesis conditions (drying and calcination) of sulfated zirconia on the final catalytic behavior of bifunctional composite catalysts prepared by the physical mixing of the sulfated zirconia (methanol dehydration catalyst) with Cu/ZnO/Al<s...

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Main Authors: Hela Lassoued, Noelia Mota, Elena Millán Ordóñez, Sahar Raissi, Mohamed Kadri Younes, Carlos Quilis Romero, Rufino M. Navarro Yerga
Format: Article
Language:English
Published: MDPI AG 2023-11-01
Series:Materials
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Online Access:https://www.mdpi.com/1996-1944/16/23/7328
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author Hela Lassoued
Noelia Mota
Elena Millán Ordóñez
Sahar Raissi
Mohamed Kadri Younes
Carlos Quilis Romero
Rufino M. Navarro Yerga
author_facet Hela Lassoued
Noelia Mota
Elena Millán Ordóñez
Sahar Raissi
Mohamed Kadri Younes
Carlos Quilis Romero
Rufino M. Navarro Yerga
author_sort Hela Lassoued
collection DOAJ
description This work is dedicated to the study of the effect of the synthesis conditions (drying and calcination) of sulfated zirconia on the final catalytic behavior of bifunctional composite catalysts prepared by the physical mixing of the sulfated zirconia (methanol dehydration catalyst) with Cu/ZnO/Al<sub>2</sub>O<sub>3</sub> (CZA; methanol synthesis catalyst). The main objective was to optimize the CZA-ZrO<sub>2</sub>/SO<sub>4</sub><sup>2−</sup> composite catalyst for its use in the direct production of dimethyl ether (DME) from syngas. Sulfated zirconia aerogel (AZS) and xerogel (XZS) were prepared using the sol–gel method using different solvent evacuation conditions and calcination temperatures, while the Cu-ZnO(Al) catalyst was synthesized using the coprecipitation procedure. The effectivity of CZA-ZrO<sub>2</sub>/SO<sub>4</sub><sup>2−</sup> composite catalysts for the direct production of dimethyl ether (DME) from syngas was evaluated in a flow reactor at 250 °C and 30 bar total pressure. The characterization of the sulfated zirconia aerogels and xerogels using different techniques showed that the mesoporous aerogel (AZS<sub>0.5</sub>300) exhibited the best textural and acidic properties due to the gel drying under supercritical conditions and calcination at 300 °C. As a result, the composite catalyst CZA-AZS<sub>0.5</sub>300 exhibited seven times higher DME production than its xerogel-containing counterpart (364 vs. 52 μmol<sub>DME</sub>·min<sup>−1</sup>·g<sub>cat</sub><sup>−1</sup>). This was attributed to its well-matched metal surface, mesoporous structure, optimal crystallite size and, most importantly, its higher acidity.
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spelling doaj.art-d5baf2146ab546528019ebf3b7cacc9e2023-12-08T15:20:45ZengMDPI AGMaterials1996-19442023-11-011623732810.3390/ma16237328Improved Dimethyl Ether Production from Syngas over Aerogel Sulfated Zirconia and Cu-ZnO(Al) Bifunctional Composite CatalystsHela Lassoued0Noelia Mota1Elena Millán Ordóñez2Sahar Raissi3Mohamed Kadri Younes4Carlos Quilis Romero5Rufino M. Navarro Yerga6Laboratory of Material Chemistry and Catalysis, Department of Chemistry, Faculty of Sciences of Tunis, University of Tunis El Manar, Tunis 2092, TunisiaInstituto de Catálisis y Petroleoquímica (CSIC), c/Marie Curie 2, Cantoblanco, 28049 Madrid, SpainInstituto de Catálisis y Petroleoquímica (CSIC), c/Marie Curie 2, Cantoblanco, 28049 Madrid, SpainLaboratory of Material Chemistry and Catalysis, Department of Chemistry, Faculty of Sciences of Tunis, University of Tunis El Manar, Tunis 2092, TunisiaLaboratory of Material Chemistry and Catalysis, Department of Chemistry, Faculty of Sciences of Tunis, University of Tunis El Manar, Tunis 2092, TunisiaInstituto de Catálisis y Petroleoquímica (CSIC), c/Marie Curie 2, Cantoblanco, 28049 Madrid, SpainInstituto de Catálisis y Petroleoquímica (CSIC), c/Marie Curie 2, Cantoblanco, 28049 Madrid, SpainThis work is dedicated to the study of the effect of the synthesis conditions (drying and calcination) of sulfated zirconia on the final catalytic behavior of bifunctional composite catalysts prepared by the physical mixing of the sulfated zirconia (methanol dehydration catalyst) with Cu/ZnO/Al<sub>2</sub>O<sub>3</sub> (CZA; methanol synthesis catalyst). The main objective was to optimize the CZA-ZrO<sub>2</sub>/SO<sub>4</sub><sup>2−</sup> composite catalyst for its use in the direct production of dimethyl ether (DME) from syngas. Sulfated zirconia aerogel (AZS) and xerogel (XZS) were prepared using the sol–gel method using different solvent evacuation conditions and calcination temperatures, while the Cu-ZnO(Al) catalyst was synthesized using the coprecipitation procedure. The effectivity of CZA-ZrO<sub>2</sub>/SO<sub>4</sub><sup>2−</sup> composite catalysts for the direct production of dimethyl ether (DME) from syngas was evaluated in a flow reactor at 250 °C and 30 bar total pressure. The characterization of the sulfated zirconia aerogels and xerogels using different techniques showed that the mesoporous aerogel (AZS<sub>0.5</sub>300) exhibited the best textural and acidic properties due to the gel drying under supercritical conditions and calcination at 300 °C. As a result, the composite catalyst CZA-AZS<sub>0.5</sub>300 exhibited seven times higher DME production than its xerogel-containing counterpart (364 vs. 52 μmol<sub>DME</sub>·min<sup>−1</sup>·g<sub>cat</sub><sup>−1</sup>). This was attributed to its well-matched metal surface, mesoporous structure, optimal crystallite size and, most importantly, its higher acidity.https://www.mdpi.com/1996-1944/16/23/7328DMEsyngasdirect synthesisCu-ZnOsulfated zirconiasol gel
spellingShingle Hela Lassoued
Noelia Mota
Elena Millán Ordóñez
Sahar Raissi
Mohamed Kadri Younes
Carlos Quilis Romero
Rufino M. Navarro Yerga
Improved Dimethyl Ether Production from Syngas over Aerogel Sulfated Zirconia and Cu-ZnO(Al) Bifunctional Composite Catalysts
Materials
DME
syngas
direct synthesis
Cu-ZnO
sulfated zirconia
sol gel
title Improved Dimethyl Ether Production from Syngas over Aerogel Sulfated Zirconia and Cu-ZnO(Al) Bifunctional Composite Catalysts
title_full Improved Dimethyl Ether Production from Syngas over Aerogel Sulfated Zirconia and Cu-ZnO(Al) Bifunctional Composite Catalysts
title_fullStr Improved Dimethyl Ether Production from Syngas over Aerogel Sulfated Zirconia and Cu-ZnO(Al) Bifunctional Composite Catalysts
title_full_unstemmed Improved Dimethyl Ether Production from Syngas over Aerogel Sulfated Zirconia and Cu-ZnO(Al) Bifunctional Composite Catalysts
title_short Improved Dimethyl Ether Production from Syngas over Aerogel Sulfated Zirconia and Cu-ZnO(Al) Bifunctional Composite Catalysts
title_sort improved dimethyl ether production from syngas over aerogel sulfated zirconia and cu zno al bifunctional composite catalysts
topic DME
syngas
direct synthesis
Cu-ZnO
sulfated zirconia
sol gel
url https://www.mdpi.com/1996-1944/16/23/7328
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