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Quantitative screening of an extended oxidative coupling of methane catalyst library
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Alexiadis, V. I., Chaar, M., van Veen, André C., Muhler, M., Thybaut, J. W. and Marin, G. B. (2016) Quantitative screening of an extended oxidative coupling of methane catalyst library. Applied Catalysis B: Environmental, 199 . pp. 252-259. doi:10.1016/j.apcatb.2016.06.019
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WRAP-quantitative-screening-extended-oxidative-coupling-methane-van-Veen-2017.pdf - Published Version - Requires a PDF viewer. Available under License Creative Commons Attribution Non-commercial No Derivatives 4.0. Download (1600Kb) | Preview |
Official URL: http://dx.doi.org/10.1016/j.apcatb.2016.06.019
Abstract
A comprehensive microkinetic model, including catalyst descriptors, that accounts for the homogeneous as well as heterogeneously catalyzed reaction steps in Oxidative Coupling of Methane (OCM) was used in the assessment of large kinetic datasets acquired on five different catalytic materials. The applicability of the model was extended from alkali magnesia catalysts represented by Li/MgO and Sn-Li/MgO and alkaline earth lanthana catalysts represented by Sr/La2O3 to rare earth-promoted alkaline earth calcium oxide catalysts, represented by LaSr/CaO, and to a Na-Mn-W/SiO2 catalyst. The model succeeded in adequately simulating the performance of all five investigated catalysts in terms of reactant conversion and product selectivities in the entire range of experimental conditions. It was found that the activity of Sr/La2O3, in terms of methane conversion, is approximately 2, 5, 30 and 33 times higher than over the La-Sr/CaO, Sn-Li/MgO, Na-Mn-W/SiO2 and Li/MgO catalysts, respectively, under identical operating conditions. This was attributed mainly to the high stability of adsorbed hydroxyls, the high stability of adsorbed oxygen and the high concentration of active sites of Sr/La2O3. The selectivity towards C2 products was found to depend on the methyl radical sticking coefficient and the stability of the adsorbed oxygen and was the highest on the Na-W-Mn/SiO2 catalyst, that is 75% at about 1% methane conversion and 1023 K, 190 kPa and inlet molar CH4/O2 ratio of 4.
| Item Type: | Journal Article | ||||||||
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| Subjects: | T Technology > TD Environmental technology. Sanitary engineering | ||||||||
| Divisions: | Faculty of Science > Engineering | ||||||||
| Library of Congress Subject Headings (LCSH): | Ethylene, Methane, Catalysis | ||||||||
| Journal or Publication Title: | Applied Catalysis B: Environmental | ||||||||
| Publisher: | Elsevier BV | ||||||||
| ISSN: | 0926-3373 | ||||||||
| Official Date: | 15 December 2016 | ||||||||
| Dates: |
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| Date of first compliant deposit: | 20 October 2017 | ||||||||
| Volume: | 199 | ||||||||
| Page Range: | pp. 252-259 | ||||||||
| DOI: | 10.1016/j.apcatb.2016.06.019 | ||||||||
| Status: | Peer Reviewed | ||||||||
| Publication Status: | Published | ||||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||||
| Funder: | Seventh Framework Programme (European Commission) (FP7) | ||||||||
| Grant number: | Grant No. 228953 Grant No. 615456 i-CaD. (FP7) |
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