Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio

The dry and oxidative dry reforming of CH4 over alumina-supported CoeNi catalysts were investigated over 72-h longevity experiments. The deactivation behaviour at low CO2:CH4 ratio (2) suggests that carbon deposition proceeds via a rapid dehydropolymerisation step resulting in the blockage of activ...

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Main Authors: Foo, Say Yei, Cheng, C. K., Nguyen, Tuan-Huy, Adesina, Adesoji A.
Format: Article
Published: Elsevier 2012
Subjects:
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author Foo, Say Yei
Cheng, C. K.
Nguyen, Tuan-Huy
Adesina, Adesoji A.
author_facet Foo, Say Yei
Cheng, C. K.
Nguyen, Tuan-Huy
Adesina, Adesoji A.
author_sort Foo, Say Yei
collection UMP
description The dry and oxidative dry reforming of CH4 over alumina-supported CoeNi catalysts were investigated over 72-h longevity experiments. The deactivation behaviour at low CO2:CH4 ratio (2) suggests that carbon deposition proceeds via a rapid dehydropolymerisation step resulting in the blockage of active sites and loss in CO2 consumption. In particular, at high temperatures of 923 K and 973 K, a ‘breakthrough’ point was observed in which deactivation that was previously slow suddenly accelerated, indicating rapid polymerisation of deposited carbon. Only with feed CO2:CH4 > 2 or with O2 co-feeding was coke-induced deactivation eliminated. In particular, O2 co-feeding gave improved carbon removal, product H2:CO ratios more suitable for downstream GTL processing and stable catalytic performance. Conversion-time data were adequately fitted to the generalised Levenspiel reaction-deactivation model. Activation energy estimate (66e129 kJ mol1) was dependent on the CO2:CH4 ratio but representative of other hydrocarbon reforming reactions on Nibased catalysts.
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spelling UMPir67882018-01-11T03:52:21Z http://umpir.ump.edu.my/id/eprint/6788/ Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio Foo, Say Yei Cheng, C. K. Nguyen, Tuan-Huy Adesina, Adesoji A. QD Chemistry The dry and oxidative dry reforming of CH4 over alumina-supported CoeNi catalysts were investigated over 72-h longevity experiments. The deactivation behaviour at low CO2:CH4 ratio (2) suggests that carbon deposition proceeds via a rapid dehydropolymerisation step resulting in the blockage of active sites and loss in CO2 consumption. In particular, at high temperatures of 923 K and 973 K, a ‘breakthrough’ point was observed in which deactivation that was previously slow suddenly accelerated, indicating rapid polymerisation of deposited carbon. Only with feed CO2:CH4 > 2 or with O2 co-feeding was coke-induced deactivation eliminated. In particular, O2 co-feeding gave improved carbon removal, product H2:CO ratios more suitable for downstream GTL processing and stable catalytic performance. Conversion-time data were adequately fitted to the generalised Levenspiel reaction-deactivation model. Activation energy estimate (66e129 kJ mol1) was dependent on the CO2:CH4 ratio but representative of other hydrocarbon reforming reactions on Nibased catalysts. Elsevier 2012 Article PeerReviewed Foo, Say Yei and Cheng, C. K. and Nguyen, Tuan-Huy and Adesina, Adesoji A. (2012) Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio. International Journal of Hydrogen Energy, 37 (22). 17019 -17026. ISSN 0360-3199. (Published) http://dx.doi.org/10.1016/j.ijhydene.2012.08.136 doi: 10.1016/j.ijhydene.2012.08.136
spellingShingle QD Chemistry
Foo, Say Yei
Cheng, C. K.
Nguyen, Tuan-Huy
Adesina, Adesoji A.
Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio
title Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio
title_full Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio
title_fullStr Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio
title_full_unstemmed Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio
title_short Syngas Production from CH4 Dry Reforming Over Coeni/Al2O3 Catalyst: Coupled Reaction-Deactivation Kinetic Analysis and the Effect of O2 Co-Feeding on H2:CO Ratio
title_sort syngas production from ch4 dry reforming over coeni al2o3 catalyst coupled reaction deactivation kinetic analysis and the effect of o2 co feeding on h2 co ratio
topic QD Chemistry
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