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固态研磨-燃烧法制CuO-ZnO-ZrO_2/HZSM-5二甲醚合成催化剂 被引量:8

Preparation of CuO-ZnO-ZrO_2/HZSM-5 Catalysts for Synthesis of Dimethyl Ether by Solid Grinding-Combustion Method
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摘要 以柠檬酸为燃烧剂,采用固态研磨-燃烧法和机械混合法制备了CuO-ZnO-ZrO2/HZSM-5CO2加氢一步合成二甲醚双功能催化剂.采用固定床反应器,在反应温度270℃、压力为3.0 MPa、空速4 200 h-1条件下,考察了催化剂对CO2加氢一步合成二甲醚的反应性能,并采用XRD、BET、H2-TPR、NH3-TPD及XPS对催化剂的结构进行了表征.评价结果表明:随柠檬酸量的增加,二甲醚选择性和收率呈峰形变化趋势;当柠檬酸的量等于化学计量比的100%时,制备的催化剂具有较好的催化性能:CO2单程转化率为24.8%、二甲醚(DME)的选择性和收率分别为35.3%和8.7%.表征结果表明:柠檬酸的量影响催化剂的比表面积、还原性能以及CuO和ZnO的晶粒尺寸等,进而影响催化剂反应性能. Cu-ZnO-ZrO2/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from hydrogenation of COs were prepared by solid grinding-burning and mechanical mixing method. The catalyst performance of the catalyst in the hydrogenation were investigated, at reaction temperature 270 ℃, pressure of 3.0 MPa, space velocity 4 200 h-1 over a fixed-bed reactor. This article focuses on the effects of the amount of citric acid added on the catalyst struc- ture and performance. Experimental results showed that dimethyl ether selectivity and yield first increased and then decreased with the increase of citric acid, the maximum catalytic activity was obtained f~'om the catalyst prepared with the stoichiometric amount of citric acid. The one way conversion of CO2 was 24.8% , the selectivity and the yield of dimethyl ether were 35.3% and 8.7% respectively. XRD, BET, HE-TPR, NHa-TPD, XPS characteriza- tion results showed that the amount of citric acid added could influence the catalyst surface area, distribution of copper, reduction performance, consequently the catalytic performance was affected by those parameters.
出处 《分子催化》 EI CAS CSCD 北大核心 2013年第5期445-451,共7页 Journal of Molecular Catalysis(China)
基金 辽宁省科技厅工业攻关项目(No.2007223016) 辽宁省教育厅项目(No.L2013161)
关键词 固态研磨-燃烧法 柠檬酸 二甲醚 二氧化碳加氢 CuO—ZnO—ZrO2 HZSM-5 solid ground-combustion method citric acid dimethyl ether hydrogenation of carbon dioxide CuO-ZnO-ZrO2/HZSM-5
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