咪唑改性HZSM-5分子筛的制备及其催化CO2加氢合成二甲醚
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Q013; TQ032

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国家自然科学基金;甘肃省基础研究基金


Preparation of Imidazole-Modified HZSM-5 Zeolite and Its Application in Catalytic Synthesis of Dimethyl Ether from Hydrogenation of Carbon Dioxide
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    摘要:

    以咪唑为添加剂,四丙基氢氧化铵为模板剂,采用水热法制备了咪唑改性HZSM-5型分子筛, 用XRD、SEM、EDS、BET、TG和NH3-TPD等手段对合成的分子筛进行了表征,结果表明当在制备分子筛的前驱液中加入少量咪唑时,制备的HZSM-5型分子筛粒径明显减小且分布更加均匀,酸性增强,并具有更好的抗高温性能. 采用浸渍法制备了CuO-ZnO-Al2O3/咪唑改性HZSM-5双功能催化剂,探讨了其催化二氧化碳加氢制备二甲醚的活性,在反应温度270 癈、反应压力3.0 MPa、CO2 : H2 = 1 : 3(体积比)、CuO : ZnO = 2 : 1(摩尔比)和CuO-ZnO2-Al2O3 : 咪唑改性HZSM-5 = 2 : 1(质量比)的条件下,CO2的单程转化率和二甲醚的选择性分别达到了42.3 %和33.1 %.

    Abstract:

    Imidazole modified HZSM-5 zeolite was prepared using tetrapropylammoniuhydroxide as template and imidazole as additive by hydrothermal synthesis method. The samples were characterized by the methods of XRD, SEM, EDS, BET, TG and NH3-TPD. The results show that adding a small amount of imidazole can produce uniform and smaller HZSM-5 zeolite particles with higher acidity and perfect resistance to high temperature performance. The CuO-ZnO-Al2O3/imidazole-modified-HZSM-5 bifunctional catalyst was prepared by impregnation method and its catalytic activity for hydrogenation of carbon dioxide to dimethyl ether was investigated. Under reaction pressure at 3.0 MPa, space velocity (SV) at 1800 mL?gcat-1?h-1, volume ratio to CO2/H2 at 1 : 3, temperature at 270 癈, molar ratio to CuO/ZnO at 2 : 1 and weight ratio to CuO-ZnO-Al2O3/imidazole-modified-HZSM-5 at 2 : 1, the conversion of CO2 and selectivity of dimethyl ether can be reached to 46.5 % and 37.8 %, respectively.

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田海锋,杨爱梅,查飞,常玥.咪唑改性HZSM-5分子筛的制备及其催化CO2加氢合成二甲醚[J].精细化工,2014,31(2):

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  • 收稿日期:2013-09-16
  • 最后修改日期:2013-11-07
  • 录用日期:2013-11-08
  • 在线发布日期: 2014-02-08
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