High-temperature parallel screening of catalysts for the oxidative coupling of methane |
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Authors: | Louis Olivier Stphane Haag Helmut Pennemann Christian Hofmann Claude Mirodatos Andre C van Veen |
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Affiliation: | aUniversity of Lyon, Institut de Recherches sur la Catalyse et l’Environnement de Lyon (UMR 5256, CNRS – Université Claude Bernard Lyon 1), 2 avenue Albert Einstein, 69626 Villeurbanne Cedex, France;bInstitut für Mikrotechnik Mainz GmbH, Carl-Zeiss-Straße 18-20, 55129 Mainz, Germany |
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Abstract: | The oxidative coupling of methane (OCM) was investigated with a specifically designed multi-channel device operating fixed-bed reactors at high temperature and atmospheric pressure. The device allows precise temperature measurement in each channel selected for analysis and possesses a quench cooling unit right after the reaction zone. Analysis is based on a mass spectrometer allowing a time resolution of only 3 s per analysis and 30 s per reactor channel. Successful screening is demonstrated using a reactant feed of O2 and CH4 diluted in Ar at flows between 100 and 166 mL/min per reactor channel. As expected, Li/MgO-based catalysts showed good initial performance, but rapid deactivation at 800 °C excludes their use in high-temperature applications. Good C2 selectivity up to 80% and high yields up to 20% were observed for La/Sr/CaO catalysts. Even more interesting, no decline in performance was observed for those formulations identifying 10% La/20% Sr/CaO as best catalyst in an initial library. Screening of various La and Sr loadings at different operating conditions identified a optimal content of 5–10% for La and 20% for Sr. The exploration of operating conditions showed increasing C2 productivities with increasing reactant partial pressure, reaching at 800 °C values up to 1.3 × 10−5 mol (C2) s−1 g(cat)−1. |
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Keywords: | Parallel reactor OCM Temperature stability Reactor design |
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