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Boreskov Institute of Catalysis of the Siberian Branch of Russian ...

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OP-IV-3CO REMOVAL FROM H 2 -rich GAS MIXTURES IN MICROCHANNELREACTORS WITH Cu/CeO 2-x CATALYSTSP.V. Snytnikov 1,2 , Y. Men 3 , V. Hessel 3,4 , V.A. Sobyanin 1,21 <strong>Boreskov</strong> <strong>Institute</strong> <strong>of</strong> <strong>Catalysis</strong> SB RAS, Pr. Lavrentieva, 5, Novosibirsk, 630090, RussiaE-mail: pvsnyt@catalysis.ru2 Novosibirsk State University, Pirogova St., 2, Novosibirsk, 630090, Russia3 Institut fur Mikrotechnik Mainz GmbH, Carl-Zeiss-Strasse 18-20, Mainz, 55129, Germany4 Eindhoven University <strong>of</strong> Technology, Den Doleh, 2, Eindhoven, 5600 MB, <strong>the</strong> Ne<strong>the</strong>rlandsPreferential CO oxidation (PROX) is one <strong>of</strong> <strong>the</strong> promising methods for CO removal fromhydrogen-rich gas mixtures produced by hydrocarbons conversion processes. Microchanneldesign <strong>of</strong> catalytic reactors due to enhanced heat and mass transfer has big advantages for thisprocess. However it requires development <strong>of</strong> new active components <strong>of</strong> catalysts able torealize <strong>the</strong>se engineering breakthroughs by operation at short contact times without loss <strong>of</strong>activity and stability. Besides such engineering arguments, micro-channel reactors demand fornew kinds <strong>of</strong> catalyst formulation also from <strong>the</strong> system integration side, most prominentlybeing washcoated layers attached to <strong>the</strong> channels’ walls.Several series <strong>of</strong> <strong>the</strong> catalysts for preferential CO oxidation were syn<strong>the</strong>sized. Copperceriumoxide was used as <strong>the</strong> main active component. The catalysts were syn<strong>the</strong>sized byvarious procedures that allowed variation <strong>of</strong> <strong>the</strong> textural and morphological characteristics <strong>of</strong><strong>the</strong> samples. The main efforts were focused on <strong>the</strong> finding <strong>of</strong> <strong>the</strong> optimum copper-ceriumoxide catalyst composition and development <strong>of</strong> <strong>the</strong> most feasible preparation procedure thatwould provide introduction <strong>of</strong> <strong>the</strong> active component into microchannels without activitylosses. It was obtained that <strong>the</strong> procedure for copper-ceria catalyst introduction intomicrochannels based on <strong>the</strong> deposition <strong>of</strong> water suspension <strong>of</strong> <strong>the</strong> catalyst with polyvinylalcohol as a binder was <strong>the</strong> most promising one. Experiments with <strong>the</strong> variation <strong>of</strong> catalystcomposition and preparation method <strong>of</strong> catalyst-binder suspension resulted in reproducibledata on <strong>the</strong> introduction <strong>of</strong> copper-cerium oxide washcoats into microchannels <strong>of</strong> stainlesssteel platelets. The obtained samples demonstrated good impact-resistance, survived contactswith water (that is critically important for microreactor operation in real conditions, as well asin <strong>the</strong> case <strong>of</strong> water condensing on fuel processor startup and stop).Simple sandwiched (two-plate) and laserwelded micro-channel reactors were used forcatalyst testing. The catalyst performance for selective CO oxidation in H 2 excess was studiedin a flow setup with on-line chromatographic analysis <strong>of</strong> <strong>the</strong> reaction products. Catalyticperformance <strong>of</strong> <strong>the</strong> microchannel reactors were checked using model feeds at WHSV =5000 ÷ 120000 cm 3 /g·h and temperature 100 ÷ 300 °С. For comparative experiments on <strong>the</strong>activity <strong>of</strong> copper-cerium oxide catalyst towards <strong>the</strong> reactions in <strong>the</strong> microreactor and in144

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