Oxidative Coupling of Methane over Pt/Al<sub>2</sub>O<sub>3</sub> at High Temperature: Multiscale Modeling of the Catalytic Monolith
At high temperatures, the oxidative coupling of methane (OCM) is an attractive approach for catalytic conversion of methane into value-added chemicals. Experiments with a Pt/Al<sub>2</sub>O<sub>3</sub>-coated catalytic honeycomb monolith were conducted with varying CH<sub&...
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MDPI AG
2022-02-01
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| Series: | Catalysts |
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| Online Access: | https://www.mdpi.com/2073-4344/12/2/189 |
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| author | Jaspreet Chawla Sven Schardt Sofia Angeli Patrick Lott Steffen Tischer Lubow Maier Olaf Deutschmann |
| author_facet | Jaspreet Chawla Sven Schardt Sofia Angeli Patrick Lott Steffen Tischer Lubow Maier Olaf Deutschmann |
| author_sort | Jaspreet Chawla |
| collection | DOAJ |
| description | At high temperatures, the oxidative coupling of methane (OCM) is an attractive approach for catalytic conversion of methane into value-added chemicals. Experiments with a Pt/Al<sub>2</sub>O<sub>3</sub>-coated catalytic honeycomb monolith were conducted with varying CH<sub>4</sub>/O<sub>2</sub> ratios, N<sub>2</sub> dilution at atmospheric pressure, and very short contact times. The reactor was modeled by a multiscale approach using a parabolic two-dimensional flow field description in the monolithic channels coupled with a heat balance of the monolithic structure, and multistep surface reaction mechanisms as well as elementary-step, gas phase reaction mechanisms. The contribution of heterogeneous and homogeneous reactions, both of which are important for the optimization of C<sub>2</sub> products, is investigated using a combination of experimental and computational methods. The oxidation of methane, which takes place over the platinum catalyst, causes the adiabatic temperature increase required for the generation of CH<sub>3</sub> radicals in the gas phase, which are essential for the formation of C<sub>2</sub> species. Lower CH<sub>4</sub>/O<sub>2</sub> ratios result in higher C<sub>2</sub> selectivity. However, the presence of OH radicals at high temperatures facilitates subsequent conversion of C<sub>2</sub>H<sub>2</sub> at a CH<sub>4</sub>/O<sub>2</sub> ratio of 1.4. Thereby, C<sub>2</sub> species selectivity of 7% was achieved at CH<sub>4</sub>/O<sub>2</sub> ratio of 1.6, with 35% N<sub>2</sub> dilution. |
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| language | English |
| last_indexed | 2024-03-09T22:22:22Z |
| publishDate | 2022-02-01 |
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| spelling | doaj.art-96bd2f6f2b46487ab3ee6b659af833a62023-11-23T19:12:43ZengMDPI AGCatalysts2073-43442022-02-0112218910.3390/catal12020189Oxidative Coupling of Methane over Pt/Al<sub>2</sub>O<sub>3</sub> at High Temperature: Multiscale Modeling of the Catalytic MonolithJaspreet Chawla0Sven Schardt1Sofia Angeli2Patrick Lott3Steffen Tischer4Lubow Maier5Olaf Deutschmann6Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), 76131 Karlsruhe, GermanyInstitute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), 76131 Karlsruhe, GermanyInstitute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), 76131 Karlsruhe, GermanyInstitute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), 76131 Karlsruhe, GermanyInstitute of Catalysis Research and Technology (IKFT), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, GermanyInstitute of Catalysis Research and Technology (IKFT), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, GermanyInstitute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), 76131 Karlsruhe, GermanyAt high temperatures, the oxidative coupling of methane (OCM) is an attractive approach for catalytic conversion of methane into value-added chemicals. Experiments with a Pt/Al<sub>2</sub>O<sub>3</sub>-coated catalytic honeycomb monolith were conducted with varying CH<sub>4</sub>/O<sub>2</sub> ratios, N<sub>2</sub> dilution at atmospheric pressure, and very short contact times. The reactor was modeled by a multiscale approach using a parabolic two-dimensional flow field description in the monolithic channels coupled with a heat balance of the monolithic structure, and multistep surface reaction mechanisms as well as elementary-step, gas phase reaction mechanisms. The contribution of heterogeneous and homogeneous reactions, both of which are important for the optimization of C<sub>2</sub> products, is investigated using a combination of experimental and computational methods. The oxidation of methane, which takes place over the platinum catalyst, causes the adiabatic temperature increase required for the generation of CH<sub>3</sub> radicals in the gas phase, which are essential for the formation of C<sub>2</sub> species. Lower CH<sub>4</sub>/O<sub>2</sub> ratios result in higher C<sub>2</sub> selectivity. However, the presence of OH radicals at high temperatures facilitates subsequent conversion of C<sub>2</sub>H<sub>2</sub> at a CH<sub>4</sub>/O<sub>2</sub> ratio of 1.4. Thereby, C<sub>2</sub> species selectivity of 7% was achieved at CH<sub>4</sub>/O<sub>2</sub> ratio of 1.6, with 35% N<sub>2</sub> dilution.https://www.mdpi.com/2073-4344/12/2/189oxidative coupling methanekinetic modelingplatinum catalystacetylene |
| spellingShingle | Jaspreet Chawla Sven Schardt Sofia Angeli Patrick Lott Steffen Tischer Lubow Maier Olaf Deutschmann Oxidative Coupling of Methane over Pt/Al<sub>2</sub>O<sub>3</sub> at High Temperature: Multiscale Modeling of the Catalytic Monolith Catalysts oxidative coupling methane kinetic modeling platinum catalyst acetylene |
| title | Oxidative Coupling of Methane over Pt/Al<sub>2</sub>O<sub>3</sub> at High Temperature: Multiscale Modeling of the Catalytic Monolith |
| title_full | Oxidative Coupling of Methane over Pt/Al<sub>2</sub>O<sub>3</sub> at High Temperature: Multiscale Modeling of the Catalytic Monolith |
| title_fullStr | Oxidative Coupling of Methane over Pt/Al<sub>2</sub>O<sub>3</sub> at High Temperature: Multiscale Modeling of the Catalytic Monolith |
| title_full_unstemmed | Oxidative Coupling of Methane over Pt/Al<sub>2</sub>O<sub>3</sub> at High Temperature: Multiscale Modeling of the Catalytic Monolith |
| title_short | Oxidative Coupling of Methane over Pt/Al<sub>2</sub>O<sub>3</sub> at High Temperature: Multiscale Modeling of the Catalytic Monolith |
| title_sort | oxidative coupling of methane over pt al sub 2 sub o sub 3 sub at high temperature multiscale modeling of the catalytic monolith |
| topic | oxidative coupling methane kinetic modeling platinum catalyst acetylene |
| url | https://www.mdpi.com/2073-4344/12/2/189 |
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