Deactivation of Cu/ZnO catalyst during dehydrogenation of methanol |
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Authors: | Kwang-Deog Jung Oh-Shim Joo Sung-Hwan Han Sung-Jin Uhm In-Jae Chung |
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Affiliation: | (1) Korea Institute of Science and Technology, Cheongryang, PO Box 131, Seoul, Korea;(2) Department of Chemical Engineering, Korea Advanced Institute of Science and Technology, Kusung-Dong, Yusung-Ku, Daejeon, Korea |
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Abstract: | The deactivation of Cu/ZnO catalyst during methanol dehydrogenation to form methyl formate has been studied. The Cu/ZnO catalyst was seriously deactivated under the reaction conditions: various temperatures of 493, 523 and 553 K, atmospheric pressure and methanol GHSV of 3000 ml (STP)/g-cat h. The weight loss due to reduction of ZnO in the Cu/ ZnO catalyst was monitored by a microbalance. X-ray induced Auger spectroscopy of Zn(L3M4,5M4,5) showed the increase in the concentration of metallic Zn on the catalyst surface after the reaction. Temperature-programmed reduction (TPR) of the Cu/ZnO catalyst with methanol demonstrated that the reduction of ZnO in Cu/ ZnO was suppressed by introduction of CO2 into the stream of helium-methanol. As the concentration of CO2 in the feed gas increased, the weight loss of the Cu/ZnO catalyst due to the reduction of ZnO decreased. The deactivation of the Cu/ZnO catalyst in the methanol dehydrogenation was also retarded by the addition of CO2. In particular, oxygen injection into the reactant feed regenerated the Cu/ ZnO catalyst deactivated during the reaction. Based on these observations, the cause of deactivation of the Cu/ZnO catalyst has been discussed. |
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Keywords: | methanol dehydrogenation deactivation of Cu/ZnO catalyst reduction of ZnO oxidant effect regeneration of deactivated catalyst |
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