Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts
Rising concerns about petroleum depletion and energy demand are calling for alternative processes such as methane partial oxidation to produce syngas for downstream synthetic fuel production. However, industrial application is limited by catalyst deactivation caused by carbon deposition and reoxidat...
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my.utm.953412022-04-29T22:26:37Z http://eprints.utm.my/id/eprint/95341/ Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts Tan, Ji Siang Abdul Jalil, Aishah Abdulrahman, Abdulrasheed Hambali, Hambali Umar TP Chemical technology Rising concerns about petroleum depletion and energy demand are calling for alternative processes such as methane partial oxidation to produce syngas for downstream synthetic fuel production. However, industrial application is limited by catalyst deactivation caused by carbon deposition and reoxidation of active metals. Here we synthesized dendritic fibrous Pd, Ru and Rh/KAUST Catalysis Centre 1 (KCC-1) catalysts by microemulsion followed by wetness impregnation. Catalysts were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, electronic spin resonance, Fourier transform infrared spectroscopy and UV–Vis diffuse reflectance spectroscopy. We measured catalytic performance, stability and regenerability at 900 °C over 16 h-on-stream. Results reveal that oxygen vacancies into the KCC-1 framework enhance the interaction with noble metal particles, creating a strong metal–support interaction decreasing in the order Rh/KCC-1, Pd/KCC-1, Ru/KCC-1. Interestingly, CH4 conversion followed the same order: 74-80% for Rh/KCC-1, 60-71% for Pd/KCC-1, 53-63% for Ru/KCC-1, without a significant carbon deposit. These findings mean that oxygen vacancies retained the metal in the active metallic phase and prevented carbon deposits. Overall, metal/KCC-1 is as bifunctional catalyst whereby oxygen vacancies generate labile electrons contributing to electrostatic metal–support interactions, stabilization of metal phases and providing labile oxygen ions for carbon gasification. Springer Science and Business Media Deutschland GmbH 2021 Article PeerReviewed Tan, Ji Siang and Abdul Jalil, Aishah and Abdulrahman, Abdulrasheed and Hambali, Hambali Umar (2021) Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts. Environmental Chemistry Letters, 19 (3). pp. 2733-2742. ISSN 1610-3653 http://dx.doi.org/10.1007/s10311-021-01192-0 |
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TP Chemical technology Tan, Ji Siang Abdul Jalil, Aishah Abdulrahman, Abdulrasheed Hambali, Hambali Umar Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts |
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Rising concerns about petroleum depletion and energy demand are calling for alternative processes such as methane partial oxidation to produce syngas for downstream synthetic fuel production. However, industrial application is limited by catalyst deactivation caused by carbon deposition and reoxidation of active metals. Here we synthesized dendritic fibrous Pd, Ru and Rh/KAUST Catalysis Centre 1 (KCC-1) catalysts by microemulsion followed by wetness impregnation. Catalysts were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, electronic spin resonance, Fourier transform infrared spectroscopy and UV–Vis diffuse reflectance spectroscopy. We measured catalytic performance, stability and regenerability at 900 °C over 16 h-on-stream. Results reveal that oxygen vacancies into the KCC-1 framework enhance the interaction with noble metal particles, creating a strong metal–support interaction decreasing in the order Rh/KCC-1, Pd/KCC-1, Ru/KCC-1. Interestingly, CH4 conversion followed the same order: 74-80% for Rh/KCC-1, 60-71% for Pd/KCC-1, 53-63% for Ru/KCC-1, without a significant carbon deposit. These findings mean that oxygen vacancies retained the metal in the active metallic phase and prevented carbon deposits. Overall, metal/KCC-1 is as bifunctional catalyst whereby oxygen vacancies generate labile electrons contributing to electrostatic metal–support interactions, stabilization of metal phases and providing labile oxygen ions for carbon gasification. |
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Article |
author |
Tan, Ji Siang Abdul Jalil, Aishah Abdulrahman, Abdulrasheed Hambali, Hambali Umar |
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Tan, Ji Siang Abdul Jalil, Aishah Abdulrahman, Abdulrasheed Hambali, Hambali Umar |
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Tan, Ji Siang |
title |
Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts |
title_short |
Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts |
title_full |
Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts |
title_fullStr |
Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts |
title_full_unstemmed |
Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts |
title_sort |
enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous pd, ru and rh/kcc-1 catalysts |
publisher |
Springer Science and Business Media Deutschland GmbH |
publishDate |
2021 |
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http://eprints.utm.my/id/eprint/95341/ http://dx.doi.org/10.1007/s10311-021-01192-0 |
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1732945461227028480 |