A study on highly active Cu-Zn-Al-K catalyst for CO2 hydrogenation to methanol
Excellent CO2 hydrogenation activity results were obtained on Cu-Zn-Al-K (CZA-K) catalyst with 10% of CO2 conversion and 98% of methanol selectivity at 220 °C. The CZA-K catalyst was precipitated by using 4 M K2CO3/KOH solution. For comparison purpose, CZA-Na and CZA catalysts were synthesized by us...
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Elsevier
2021-02-01
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Series: | Arabian Journal of Chemistry |
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Online Access: | http://www.sciencedirect.com/science/article/pii/S1878535220305128 |
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author | Nagaraju Pasupulety Abdurahim A. Al-Zahrani Muhammad A. Daous Seetharamulu Podila Hafedh Driss |
author_facet | Nagaraju Pasupulety Abdurahim A. Al-Zahrani Muhammad A. Daous Seetharamulu Podila Hafedh Driss |
author_sort | Nagaraju Pasupulety |
collection | DOAJ |
description | Excellent CO2 hydrogenation activity results were obtained on Cu-Zn-Al-K (CZA-K) catalyst with 10% of CO2 conversion and 98% of methanol selectivity at 220 °C. The CZA-K catalyst was precipitated by using 4 M K2CO3/KOH solution. For comparison purpose, CZA-Na and CZA catalysts were synthesized by using 4 M solutions of Na2CO3/NaOH and (NH4)2CO3/NH4OH respectively. Characterization of these catalysts was done by using BET-poresize, XRD, FTIR-DRIFTs, high pressure-TPR, CO2-TPD-mass, XPS and HAADF-STEM-EDX techniques. Among the catalysts studied maximum methanol space time yield of 14.4 mmol·gcat−·h− was obtained on CZA-K at 240 °C with 2400 h− GHSV of CO2/H2 mole ratio equals to 1:4. Greater methanol yield was associated with superior surface Cu+/Cu0 content in CZA-K was obtained through K2CO3/KOH precipitation. Further, FTIR-DRIFTs spectra suggests the interaction of CO2 with the potassium existed in the CZA framework (0.65% K, EDX) led to the formation of KO(CO)O surface species. To some extent, CO2 dissociation to CO and subsequent CH4 formation was limited by this species in presence of H2. At 240 °C, steady catalytic activity was observed for 100 h of continuous operation on CZA-K. It was associated with fewer carbon deposits formation and segregated active metals in CZA-K catalyst. The decreasing order of CO2 hydrogenation activity at 240 °C with 3.0 MPa feed-gas pressure as follows: CZA-K (14% CO2 conversion and 96% methanol selectivity) > CZA-Na (11% and 94%) > CZA (9% and 92%). |
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language | English |
last_indexed | 2024-12-16T16:27:45Z |
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series | Arabian Journal of Chemistry |
spelling | doaj.art-1c9fee0b3d404298b33ae3dae4710cbe2022-12-21T22:24:42ZengElsevierArabian Journal of Chemistry1878-53522021-02-01142102951A study on highly active Cu-Zn-Al-K catalyst for CO2 hydrogenation to methanolNagaraju Pasupulety0Abdurahim A. Al-Zahrani1Muhammad A. Daous2Seetharamulu Podila3Hafedh Driss4Corresponding author.; Chemical & Materials Engineering Department, College of Engineering, King Abdulaziz University, P.O. Box 80204, Jeddah 21589, Saudi ArabiaChemical & Materials Engineering Department, College of Engineering, King Abdulaziz University, P.O. Box 80204, Jeddah 21589, Saudi ArabiaChemical & Materials Engineering Department, College of Engineering, King Abdulaziz University, P.O. Box 80204, Jeddah 21589, Saudi ArabiaChemical & Materials Engineering Department, College of Engineering, King Abdulaziz University, P.O. Box 80204, Jeddah 21589, Saudi ArabiaChemical & Materials Engineering Department, College of Engineering, King Abdulaziz University, P.O. Box 80204, Jeddah 21589, Saudi ArabiaExcellent CO2 hydrogenation activity results were obtained on Cu-Zn-Al-K (CZA-K) catalyst with 10% of CO2 conversion and 98% of methanol selectivity at 220 °C. The CZA-K catalyst was precipitated by using 4 M K2CO3/KOH solution. For comparison purpose, CZA-Na and CZA catalysts were synthesized by using 4 M solutions of Na2CO3/NaOH and (NH4)2CO3/NH4OH respectively. Characterization of these catalysts was done by using BET-poresize, XRD, FTIR-DRIFTs, high pressure-TPR, CO2-TPD-mass, XPS and HAADF-STEM-EDX techniques. Among the catalysts studied maximum methanol space time yield of 14.4 mmol·gcat−·h− was obtained on CZA-K at 240 °C with 2400 h− GHSV of CO2/H2 mole ratio equals to 1:4. Greater methanol yield was associated with superior surface Cu+/Cu0 content in CZA-K was obtained through K2CO3/KOH precipitation. Further, FTIR-DRIFTs spectra suggests the interaction of CO2 with the potassium existed in the CZA framework (0.65% K, EDX) led to the formation of KO(CO)O surface species. To some extent, CO2 dissociation to CO and subsequent CH4 formation was limited by this species in presence of H2. At 240 °C, steady catalytic activity was observed for 100 h of continuous operation on CZA-K. It was associated with fewer carbon deposits formation and segregated active metals in CZA-K catalyst. The decreasing order of CO2 hydrogenation activity at 240 °C with 3.0 MPa feed-gas pressure as follows: CZA-K (14% CO2 conversion and 96% methanol selectivity) > CZA-Na (11% and 94%) > CZA (9% and 92%).http://www.sciencedirect.com/science/article/pii/S1878535220305128CO2 hydrogenationMethanol and Cu-Zn-Al-K catalyst |
spellingShingle | Nagaraju Pasupulety Abdurahim A. Al-Zahrani Muhammad A. Daous Seetharamulu Podila Hafedh Driss A study on highly active Cu-Zn-Al-K catalyst for CO2 hydrogenation to methanol Arabian Journal of Chemistry CO2 hydrogenation Methanol and Cu-Zn-Al-K catalyst |
title | A study on highly active Cu-Zn-Al-K catalyst for CO2 hydrogenation to methanol |
title_full | A study on highly active Cu-Zn-Al-K catalyst for CO2 hydrogenation to methanol |
title_fullStr | A study on highly active Cu-Zn-Al-K catalyst for CO2 hydrogenation to methanol |
title_full_unstemmed | A study on highly active Cu-Zn-Al-K catalyst for CO2 hydrogenation to methanol |
title_short | A study on highly active Cu-Zn-Al-K catalyst for CO2 hydrogenation to methanol |
title_sort | study on highly active cu zn al k catalyst for co2 hydrogenation to methanol |
topic | CO2 hydrogenation Methanol and Cu-Zn-Al-K catalyst |
url | http://www.sciencedirect.com/science/article/pii/S1878535220305128 |
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