Catalytic Conversion of Chloromethane to Olefins and Aromatics Over Zeolite Catalysts
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Catalytic Conversion of Chloromethane to Olefins and Aromatics Over Zeolite Catalysts Di Zhu1 · Zi Wang2 · Fei Meng2 · Baofeng Zhao1 · Swarom Kanitkar3 · Yongchun Tang2 Received: 5 June 2020 / Accepted: 21 August 2020 © Springer Science+Business Media, LLC, part of Springer Nature 2020
Abstract We report the tunable conversion of chloromethane to olefins and aromatics using different metal-promoted zeolites as catalysts. Despite SAPO-34 was industrially used as catalysts for methanol to olefins reaction (MTO), the SAPO-34 based zeolites exhibited low activity and short lifetime when using chloromethane as the feed. Higher chloromethane conversion and longer catalyst lifetime were found on H-ZSM-5. The activity and product distribution can be improved by optimizing the reaction temperature and space velocity. Impregnating the H-ZSM-5 zeolite with 1 wt% and 5 wt% metal oxide as promoters significantly enhanced the conversion efficiency and altered the product distribution. The highest aromatics selectivity (38%) was obtained on the H-ZSM-5 zeolite promoted by 5 wt% Ni, whereas on 5 wt% Mg and 5 wt% Mn promoted H-ZSM-5, the aromatics selectivity is merely 5%. Therefore, different modified H-ZSM-5 could be used to convert chloromethane to either aromatics or olefin-heavy products. It was found that the aromatics yield is strongly correlated to the acidity of the H-ZSM-5 zeolite.
Di Zhu and Zi Wang have contributed equally to this study. Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10562-020-03364-z) contains supplementary material, which is available to authorized users. * Zi Wang [email protected] 1
Key Laboratory for Biomass Gasification Technology of Shandong Province, Energy Research Institute, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250014, China
2
Power Environmental Energy Research Institute, 738 Arrow Grand Circle, Covina, CA 91722, USA
3
Department of Chemical Engineering, Louisiana State University, Baton Rouge, LA 70803, USA
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Graphic Abstract
Keywords Chloromethane · H-ZSM-5 · SAPO-34 · Olefins · Aromatics
1 Introduction With the abundant reserves and desirable carbon-hydrogen ratio, methane (CH4), the major component of shale gas, is a promising starting material to synthesize important industrial chemical intermediates such as light olefins(C2–C4) and aromatics (benzene, toluene and xylene). Currently the only industrial approach to convert methane is through the syngas route, which demand high operating temperature and capital cost. On the other hand, the direct methane conversion processes are potentially more cost-effective and environmentally friendly than the syngas route. These methods include pyrolysis [1, 2], oxidative coupling of methane [3], superacid catalysis [4, 5], halogenation [6, 7], etc. Among all these processes, the conversion of methane to chloromethane (CH3Cl) has been drawing increasing attention since the temperature requirement is much less
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