Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals

Carbon dioxide levels in atmosphere are linked with a number of adverse environmental impacts including climate change. CO2 utilization is one of the available technologies to reduce CO2 emissions released into atmosphere by its conversion into value added products. Hydrogenation of CO2 into hydroca...

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Main Author: Alkhalaf, Ahmed S.
Other Authors: Gascon, Jorge
Language:en
Published: 2020
Subjects:
Online Access:Alkhalaf, A. S. (2020). Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals. KAUST Research Repository. https://doi.org/10.25781/KAUST-73Z6U
http://hdl.handle.net/10754/664246
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spelling ndltd-kaust.edu.sa-oai-repository.kaust.edu.sa-10754-6642462021-02-20T17:09:18Z Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals Alkhalaf, Ahmed S. Gascon, Jorge Physical Science and Engineering (PSE) Division Sarathy, Mani Huang, Kuo-Wei CO2 Conversion Zeolite Beta Hydrogenation Methanol Iso-paraffins Carbon dioxide levels in atmosphere are linked with a number of adverse environmental impacts including climate change. CO2 utilization is one of the available technologies to reduce CO2 emissions released into atmosphere by its conversion into value added products. Hydrogenation of CO2 into hydrocarbons (with methanol being an intermediate) can be achieved in a single-pot using bi-functional catalysis system composed of metal/metal-oxide and zeolite. In this study, activated novel indium cobalt (InCo) and zeolite beta samples (BEA) were used for the conversion of CO2 into a hydrocarbon mixture rich of iso-paraffins via methanol in a single pot. The objective was to investigate the effect of zeolite beta acidity (represented by SiO2/Al2O3 ratio) and the configuration of the reactor on the overall performance of the above mentioned bi-functional system. Three samples of zeolite beta with different SiO2/Al2O3 ratios were synthesized in-house (Beta-20, Beta-100 and Beta-300) and used along with commercial beta as methanol to hydrocarbons catalysts. XRD patterns of the synthesized samples showed that all of the obtained samples are zeolite beta with high crystallinity. Adsorption-desorption isotherms of the studied zeolites revealed micro-mesoporosity of the samples. Analysis of SEM images suggests that the particles of the studied samples are of a similar range of size (100-200 nm). Each zeolite sample was used to fill two reactor configurations: dual bed and mixed bed. Samples were tested at a temperature of 300 oC, a pressure of 50 bar and CO2:H2 ratio of 1:4 except for Beta-100 sample which was tested at a CO2:H2 ratio of 1:3. CO2 conversion is a characteristic of the methanol synthesis catalyst (InCo) and it ranged between 15% to 20% for all cases. Dimethyl ether (DME) generation in dual bed configuration was much faster and at much higher rates than in mixed bed configuration for all tested samples, indicating that mixed bed configuration is more stable for this particular system. Heavier hydrocarbons (C6 and C7) are generated in higher amounts over low acidic zeolite beta than over beta of high acidity. More acidic zeolite beta, however, was found to be more stable than beta of less acidity. 2020-07-19T05:47:54Z 2020-07-19T05:47:54Z 2020-06 Thesis Alkhalaf, A. S. (2020). Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals. KAUST Research Repository. https://doi.org/10.25781/KAUST-73Z6U 10.25781/KAUST-73Z6U http://hdl.handle.net/10754/664246 en
collection NDLTD
language en
sources NDLTD
topic CO2 Conversion
Zeolite
Beta
Hydrogenation
Methanol
Iso-paraffins
spellingShingle CO2 Conversion
Zeolite
Beta
Hydrogenation
Methanol
Iso-paraffins
Alkhalaf, Ahmed S.
Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals
description Carbon dioxide levels in atmosphere are linked with a number of adverse environmental impacts including climate change. CO2 utilization is one of the available technologies to reduce CO2 emissions released into atmosphere by its conversion into value added products. Hydrogenation of CO2 into hydrocarbons (with methanol being an intermediate) can be achieved in a single-pot using bi-functional catalysis system composed of metal/metal-oxide and zeolite. In this study, activated novel indium cobalt (InCo) and zeolite beta samples (BEA) were used for the conversion of CO2 into a hydrocarbon mixture rich of iso-paraffins via methanol in a single pot. The objective was to investigate the effect of zeolite beta acidity (represented by SiO2/Al2O3 ratio) and the configuration of the reactor on the overall performance of the above mentioned bi-functional system. Three samples of zeolite beta with different SiO2/Al2O3 ratios were synthesized in-house (Beta-20, Beta-100 and Beta-300) and used along with commercial beta as methanol to hydrocarbons catalysts. XRD patterns of the synthesized samples showed that all of the obtained samples are zeolite beta with high crystallinity. Adsorption-desorption isotherms of the studied zeolites revealed micro-mesoporosity of the samples. Analysis of SEM images suggests that the particles of the studied samples are of a similar range of size (100-200 nm). Each zeolite sample was used to fill two reactor configurations: dual bed and mixed bed. Samples were tested at a temperature of 300 oC, a pressure of 50 bar and CO2:H2 ratio of 1:4 except for Beta-100 sample which was tested at a CO2:H2 ratio of 1:3. CO2 conversion is a characteristic of the methanol synthesis catalyst (InCo) and it ranged between 15% to 20% for all cases. Dimethyl ether (DME) generation in dual bed configuration was much faster and at much higher rates than in mixed bed configuration for all tested samples, indicating that mixed bed configuration is more stable for this particular system. Heavier hydrocarbons (C6 and C7) are generated in higher amounts over low acidic zeolite beta than over beta of high acidity. More acidic zeolite beta, however, was found to be more stable than beta of less acidity.
author2 Gascon, Jorge
author_facet Gascon, Jorge
Alkhalaf, Ahmed S.
author Alkhalaf, Ahmed S.
author_sort Alkhalaf, Ahmed S.
title Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals
title_short Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals
title_full Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals
title_fullStr Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals
title_full_unstemmed Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals
title_sort effect of sio2/al2o3 ratio of zeolite beta in a bi-functional system for direct co2 hydrogenation into value added chemicals
publishDate 2020
url Alkhalaf, A. S. (2020). Effect of SiO2/Al2O3 Ratio of Zeolite Beta in a Bi-functional System for Direct CO2 Hydrogenation into Value Added Chemicals. KAUST Research Repository. https://doi.org/10.25781/KAUST-73Z6U
http://hdl.handle.net/10754/664246
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