The influence of preparation methods on the behavior of Cu-Mn/ZrO_2 methanol catalysts
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Abstract:
Cu-Mn/ZrO 2 catalysts have been prepare by oxalate gel coprecipitation as well as Na 2CO 3 coprecipitation methods, and the catalysts obtained behave remarkably different activity and selectivity for CO hydrogenation to methanols ynthesis. The catalysts prepared by oxalate gel coprecipitation perform a higher activity, its surface area and particle size are lower than those of Na 2CO 3 coprecipitation prepared catalysts. The XRD patterns exhibit a kind of complex oxide that only exists in Na 2CO 3 coprecipitation prepared catalysts. The interaction among Cu,Mn and Zr is thought to be important in the characteristics of catalysts.Keywords:
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Several series of Cu-Ce-Sn-O catalysts were prepared via the coprecipitation (CP), citrate-gel (CG), and hydrothermal (HT) method, respectively, combined with a wet impregnation process. The catalysts were characterized by means of XRD, XPS, and TPR. The catalytic behavior of the catalysts for low-temperature CO oxidation was investigated by using a microreactor-GC system. The results of catalytic activity measurements showed that the Cu-Ce-Sn-O catalysts were much more active than the CuO/CeO2 and CuO/SnO2 catalysts. The catalytic activity depended on the incorporated amounts of Sn, CuO loading, calcination temperature, preparation method, and content of highly dispersed active CuO species. The 7 wt% CuO/Ce0.2Sn0.8O2 catalysts prepared by the CP method and calcined at 650°C exhibited the highest catalytic activity, while the 7 wt%CuO/Ce0.2Sn0.8O2 catalysts prepared by the CG or HT method showed higher thermal resistance.
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The effects of various calcination conditions on the structure properties and catalytic performance in the reaction of hydrogenation of CO 2 to form methanol of the nanosized Cu/ZnO/Al 2O 3 catalysts prepared by gel oxalate co precipitation method were investigated. Combining with several modern characterization methods,the influence of calcination gaseous environment,calcination temperature and different temping rate during calcination process to the crystal size,structure and interaction among components of the catalysts were studied. The catalysts were then used in methanol synthesis from CO 2 hydrogenation. The results show that the nanosized metallic copper catalysts show excellent catalytic performance for the hydrogenation of CO 2 and calcinations conditions exhibit notable influence on the catalytic performance.
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The effect of the precipitation procedure and post-treatment to the properties of CuO-Zn()/ZrO_2 catalysts in the CO_2 hydrogenation to methanol reaction was studied systematically.The catalysts were characterized by means of N_2 absorption-desorption,XRD,SEM and H_2-TPR.The results indicated that two surface copper species with different chemical environment existed in reduced catalysts,only active copper species exhibited catalysis;in addition,the activities of the catalysts were related to their grain sizes,active surface areas and pore structures.Furthermore,CuO species with appropriate grain sizes might be the effective precursor with catalytic activity,and their reaction rule was consistent with the theory of the HCOO-Cu intermediates.
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Structure and performance of Cu/ZrO_2 catalyst for the synthesis of methanol from CO_2 hydrogenation
Cu/ZrO2 catalysts were prepared through fractional precipitation,impregnation-precipitation and solid-state reaction methods and characterized by N2 sorption,XRD,TPR,in-situ IR and XPS techniques.Their catalytic performances in methanol synthesis from CO2 hydrogenation were investigated.The results showed that the physical structure and reducibility as well as the interaction between Cu and ZrO2 of a Cu/ZrO2 catalyst are greatly affected by the preparation method.The catalytic performance of Cu/ZrO2 is mainly determined by the interaction between Cu and ZrO2 rather than by the surface area.Compared with the catalysts prepared by other methods,the Cu/ZrO2 catalyst prepared by impregnation-precipitation is provided with higher CuO dispersion and stronger interaction between Cu and ZrO2;it also exhibits higher CO2 conversion and higher methanol yield when used as catalyst in the synthesis of methanol from CO2 hydrogenation.
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