Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation
The metal-free KAUST Catalysis Center 1 (KCC-1) was synthesized through microemulsion method with microwave assistance and was assessed for methane partial oxidation (MPO) under various operating conditions. The electronic spin resonance spectroscopy, pyridine-probed infrared spectroscopy, and tempe...
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my.utm.1030812023-10-12T09:22:18Z http://eprints.utm.my/103081/ Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation Tan, Ji Siang Abdul Jalil, Aishah Shahul Hamid, Muhamed Yusuf Q Science (General) TP Chemical technology The metal-free KAUST Catalysis Center 1 (KCC-1) was synthesized through microemulsion method with microwave assistance and was assessed for methane partial oxidation (MPO) under various operating conditions. The electronic spin resonance spectroscopy, pyridine-probed infrared spectroscopy, and temperature-programmed desorption of oxygen measurement indicated that the concentration of BrØnsted acid sites and oxygen vacancies in KCC-1 were at least 2-fold higher than its counterparts, which benefited MPO activity via the promotion of adsorption and dissociation of gaseous reactants. The principal species detected by post-reaction X-ray photoelectron spectroscopy (XPS) was surface-adsorbed oxygen species; its relative percentages among all oxygen species reduced in the order spent KCC-1 (77.1%) > spent MCM-41 (Mobil Composition of Matter number 41; 41.4%) > spent SiO2 (−). The catalytic performance followed the same trend, suggesting that the surface-adsorbed oxygen species was the key factor for MPO process. Additionally, the carbon deposition rate increased in the order SiO2 (16.8 mol/gcat/s) > MCM-41 (11.7 mol/gcat/s) > KCC-1 (7.7 mol/gcat/s), consistent with the results of post-reaction Raman measurements. By coupling the in situ Fourier-transform infrared and XPS results, it is suggested that the high concentration of oxygen vacancies in KCC-1 contributed to activate the CH4 molecules on acid sites via different O∗-assisted kinetically relevant C–H bond activation mechanism for combustion-reforming pathway; meanwhile it provided an excellent adsorption-desorption cycle of O2− species to inhibit the carbon deposition, thus creating a bifunctional reaction mechanism in MPO reaction. Elsevier Ltd 2022-03 Article PeerReviewed Tan, Ji Siang and Abdul Jalil, Aishah and Shahul Hamid, Muhamed Yusuf (2022) Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation. Materials Today Chemistry, 23 (NA). pp. 1-17. ISSN 2468-5194 http://dx.doi.org/10.1016/j.mtchem.2021.100684 DOI:10.1016/j.mtchem.2021.100684 |
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Q Science (General) TP Chemical technology Tan, Ji Siang Abdul Jalil, Aishah Shahul Hamid, Muhamed Yusuf Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation |
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The metal-free KAUST Catalysis Center 1 (KCC-1) was synthesized through microemulsion method with microwave assistance and was assessed for methane partial oxidation (MPO) under various operating conditions. The electronic spin resonance spectroscopy, pyridine-probed infrared spectroscopy, and temperature-programmed desorption of oxygen measurement indicated that the concentration of BrØnsted acid sites and oxygen vacancies in KCC-1 were at least 2-fold higher than its counterparts, which benefited MPO activity via the promotion of adsorption and dissociation of gaseous reactants. The principal species detected by post-reaction X-ray photoelectron spectroscopy (XPS) was surface-adsorbed oxygen species; its relative percentages among all oxygen species reduced in the order spent KCC-1 (77.1%) > spent MCM-41 (Mobil Composition of Matter number 41; 41.4%) > spent SiO2 (−). The catalytic performance followed the same trend, suggesting that the surface-adsorbed oxygen species was the key factor for MPO process. Additionally, the carbon deposition rate increased in the order SiO2 (16.8 mol/gcat/s) > MCM-41 (11.7 mol/gcat/s) > KCC-1 (7.7 mol/gcat/s), consistent with the results of post-reaction Raman measurements. By coupling the in situ Fourier-transform infrared and XPS results, it is suggested that the high concentration of oxygen vacancies in KCC-1 contributed to activate the CH4 molecules on acid sites via different O∗-assisted kinetically relevant C–H bond activation mechanism for combustion-reforming pathway; meanwhile it provided an excellent adsorption-desorption cycle of O2− species to inhibit the carbon deposition, thus creating a bifunctional reaction mechanism in MPO reaction. |
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Article |
author |
Tan, Ji Siang Abdul Jalil, Aishah Shahul Hamid, Muhamed Yusuf |
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Tan, Ji Siang Abdul Jalil, Aishah Shahul Hamid, Muhamed Yusuf |
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Tan, Ji Siang |
title |
Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation |
title_short |
Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation |
title_full |
Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation |
title_fullStr |
Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation |
title_full_unstemmed |
Bifunctional metal-free KAUST Catalysis Center 1 (KCC-1) as highly active catalyst for syngas production via methane partial oxidation |
title_sort |
bifunctional metal-free kaust catalysis center 1 (kcc-1) as highly active catalyst for syngas production via methane partial oxidation |
publisher |
Elsevier Ltd |
publishDate |
2022 |
url |
http://eprints.utm.my/103081/ http://dx.doi.org/10.1016/j.mtchem.2021.100684 |
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1781777642188439552 |
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