Reaction Mechanism Development for Methane Steam Reforming on a Ni/Al[sub.2]O[sub.3] Catalyst
In this work, a reliable kinetic reaction mechanism was revised to accurately reproduce the detailed reaction paths of steam reforming of methane over a Ni/Al[sub.2]O[sub.3] catalyst. A steady-state fixed-bed reactor experiment and a 1D reactor catalyst model were utilized for this task. The distinc...
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Veröffentlicht in: | Catalysts 2023-05, Vol.13 (5) |
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creator | Richter, Jana Rachow, Fabian Israel, Johannes Roth, Norbert Charlafti, Evgenia Günther, Vivien Flege, Jan Ingo Mauss, Fabian |
description | In this work, a reliable kinetic reaction mechanism was revised to accurately reproduce the detailed reaction paths of steam reforming of methane over a Ni/Al[sub.2]O[sub.3] catalyst. A steady-state fixed-bed reactor experiment and a 1D reactor catalyst model were utilized for this task. The distinctive feature of this experiment is the possibility to measure the axially resolved temperature profile of the catalyst bed, which makes the reaction kinetics inside the reactor visible. This allows for understanding the actual influence of the reaction kinetics on the system; while pure gas concentration measurements at the catalytic reactor outlet show near-equilibrium conditions, the inhere presented temperature profile shows that it is insufficient to base a reaction mechanism development on close equilibrium data. The new experimental data allow for achieving much higher quality in the modeling efforts. Additionally, by carefully controlling the available active surface via dilution in the experiment, it was possible to slow down the catalyst conversion rate, which helped during the adjustment of the reaction kinetics. To assess the accuracy of the revised mechanism, a monolith experiment from the literature was simulated. The results show that the fitted reaction mechanism was able to accurately predict the experimental outcomes for various inlet mass flows, temperatures, and steam-to-carbon ratios. |
doi_str_mv | 10.3390/catal13050884 |
format | Article |
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A steady-state fixed-bed reactor experiment and a 1D reactor catalyst model were utilized for this task. The distinctive feature of this experiment is the possibility to measure the axially resolved temperature profile of the catalyst bed, which makes the reaction kinetics inside the reactor visible. This allows for understanding the actual influence of the reaction kinetics on the system; while pure gas concentration measurements at the catalytic reactor outlet show near-equilibrium conditions, the inhere presented temperature profile shows that it is insufficient to base a reaction mechanism development on close equilibrium data. The new experimental data allow for achieving much higher quality in the modeling efforts. Additionally, by carefully controlling the available active surface via dilution in the experiment, it was possible to slow down the catalyst conversion rate, which helped during the adjustment of the reaction kinetics. To assess the accuracy of the revised mechanism, a monolith experiment from the literature was simulated. The results show that the fitted reaction mechanism was able to accurately predict the experimental outcomes for various inlet mass flows, temperatures, and steam-to-carbon ratios.</description><identifier>ISSN: 2073-4344</identifier><identifier>EISSN: 2073-4344</identifier><identifier>DOI: 10.3390/catal13050884</identifier><language>eng</language><publisher>MDPI AG</publisher><subject>Analysis ; Chemical reaction, Rate of ; Methane</subject><ispartof>Catalysts, 2023-05, Vol.13 (5)</ispartof><rights>COPYRIGHT 2023 MDPI AG</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Richter, Jana</creatorcontrib><creatorcontrib>Rachow, Fabian</creatorcontrib><creatorcontrib>Israel, Johannes</creatorcontrib><creatorcontrib>Roth, Norbert</creatorcontrib><creatorcontrib>Charlafti, Evgenia</creatorcontrib><creatorcontrib>Günther, Vivien</creatorcontrib><creatorcontrib>Flege, Jan Ingo</creatorcontrib><creatorcontrib>Mauss, Fabian</creatorcontrib><title>Reaction Mechanism Development for Methane Steam Reforming on a Ni/Al[sub.2]O[sub.3] Catalyst</title><title>Catalysts</title><description>In this work, a reliable kinetic reaction mechanism was revised to accurately reproduce the detailed reaction paths of steam reforming of methane over a Ni/Al[sub.2]O[sub.3] catalyst. A steady-state fixed-bed reactor experiment and a 1D reactor catalyst model were utilized for this task. The distinctive feature of this experiment is the possibility to measure the axially resolved temperature profile of the catalyst bed, which makes the reaction kinetics inside the reactor visible. This allows for understanding the actual influence of the reaction kinetics on the system; while pure gas concentration measurements at the catalytic reactor outlet show near-equilibrium conditions, the inhere presented temperature profile shows that it is insufficient to base a reaction mechanism development on close equilibrium data. The new experimental data allow for achieving much higher quality in the modeling efforts. Additionally, by carefully controlling the available active surface via dilution in the experiment, it was possible to slow down the catalyst conversion rate, which helped during the adjustment of the reaction kinetics. To assess the accuracy of the revised mechanism, a monolith experiment from the literature was simulated. The results show that the fitted reaction mechanism was able to accurately predict the experimental outcomes for various inlet mass flows, temperatures, and steam-to-carbon ratios.</description><subject>Analysis</subject><subject>Chemical reaction, Rate of</subject><subject>Methane</subject><issn>2073-4344</issn><issn>2073-4344</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><sourceid/><recordid>eNqVT02LwjAUDOKCoh73nj9gTZtK06PoLl5UqN6kyNvsa43kQ0x2wX9vFA9enXeYxwwDM4R8pizhvGQTCQF0ytmUCZF3SD9jBR_nPM-7L3-PjLw_sYgy5SKd9kldIcignKUrlEewyhu6wH_U7mzQBtq4S3RCdJBuA4KhFUbNKNvSGAK6VpOZ3vu_nySrNw_mNZ3fy1x9GJKPBrTH0ZMHJPn-2s2X4xY0HpRtXLiAjPeLRklnsVFRnxX3ESIrBH87cAP3tFIN</recordid><startdate>20230501</startdate><enddate>20230501</enddate><creator>Richter, Jana</creator><creator>Rachow, Fabian</creator><creator>Israel, Johannes</creator><creator>Roth, Norbert</creator><creator>Charlafti, Evgenia</creator><creator>Günther, Vivien</creator><creator>Flege, Jan Ingo</creator><creator>Mauss, Fabian</creator><general>MDPI AG</general><scope/></search><sort><creationdate>20230501</creationdate><title>Reaction Mechanism Development for Methane Steam Reforming on a Ni/Al[sub.2]O[sub.3] Catalyst</title><author>Richter, Jana ; Rachow, Fabian ; Israel, Johannes ; Roth, Norbert ; Charlafti, Evgenia ; Günther, Vivien ; Flege, Jan Ingo ; Mauss, Fabian</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-gale_infotracacademiconefile_A7508882783</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Analysis</topic><topic>Chemical reaction, Rate of</topic><topic>Methane</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Richter, Jana</creatorcontrib><creatorcontrib>Rachow, Fabian</creatorcontrib><creatorcontrib>Israel, Johannes</creatorcontrib><creatorcontrib>Roth, Norbert</creatorcontrib><creatorcontrib>Charlafti, Evgenia</creatorcontrib><creatorcontrib>Günther, Vivien</creatorcontrib><creatorcontrib>Flege, Jan Ingo</creatorcontrib><creatorcontrib>Mauss, Fabian</creatorcontrib><jtitle>Catalysts</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Richter, Jana</au><au>Rachow, Fabian</au><au>Israel, Johannes</au><au>Roth, Norbert</au><au>Charlafti, Evgenia</au><au>Günther, Vivien</au><au>Flege, Jan Ingo</au><au>Mauss, Fabian</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Reaction Mechanism Development for Methane Steam Reforming on a Ni/Al[sub.2]O[sub.3] Catalyst</atitle><jtitle>Catalysts</jtitle><date>2023-05-01</date><risdate>2023</risdate><volume>13</volume><issue>5</issue><issn>2073-4344</issn><eissn>2073-4344</eissn><abstract>In this work, a reliable kinetic reaction mechanism was revised to accurately reproduce the detailed reaction paths of steam reforming of methane over a Ni/Al[sub.2]O[sub.3] catalyst. A steady-state fixed-bed reactor experiment and a 1D reactor catalyst model were utilized for this task. The distinctive feature of this experiment is the possibility to measure the axially resolved temperature profile of the catalyst bed, which makes the reaction kinetics inside the reactor visible. This allows for understanding the actual influence of the reaction kinetics on the system; while pure gas concentration measurements at the catalytic reactor outlet show near-equilibrium conditions, the inhere presented temperature profile shows that it is insufficient to base a reaction mechanism development on close equilibrium data. The new experimental data allow for achieving much higher quality in the modeling efforts. Additionally, by carefully controlling the available active surface via dilution in the experiment, it was possible to slow down the catalyst conversion rate, which helped during the adjustment of the reaction kinetics. To assess the accuracy of the revised mechanism, a monolith experiment from the literature was simulated. The results show that the fitted reaction mechanism was able to accurately predict the experimental outcomes for various inlet mass flows, temperatures, and steam-to-carbon ratios.</abstract><pub>MDPI AG</pub><doi>10.3390/catal13050884</doi></addata></record> |
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subjects | Analysis Chemical reaction, Rate of Methane |
title | Reaction Mechanism Development for Methane Steam Reforming on a Ni/Al[sub.2]O[sub.3] Catalyst |
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