稀土改性SAPO-34分子筛的制备及其在CO2加氢合成低碳烯烃中的催化性能
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Q013; TQ032

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国家自然科学基金 (No. 21161017)


Preparation of Rare Earths Modified SAPO-34 and its Catalysis Performance in Synthesis of Light Olefins from CO2 Hydrogenation
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    摘要:

    采用水热合成法分别制备了氧化钇、氧化镧和氧化铈改性的SAPO-34分子筛(M-SAPO-34,M= Y 、La、Ce),用XRD、SEM、FT-IR、BET、NH3-TPD和TG进行了表征,结果表明:稀土金属成功地引入到了分子筛骨架中,改性后的催化剂比表面积增大,粒径减小,孔径和酸性强度均有所改变。将CuO-ZnO-ZrO2与稀土改性的SAPO-34分子筛按质量比1:1机械混合制备了复合催化剂CuO-ZnO-ZrO2/M-SAPO-34,用于催化二氧化碳加氢合成低碳烯烃,在反应温度400℃,压强3.0MPa,碳氢摩尔比1:3,空速1800 mL/(gcat •h),复合催化剂用量为1.0g时,CuO-ZnO-ZrO2/La-SAPO-34显示了良好的催化活性,二氧化碳的单程转化率为49.7%,低碳烯烃的选择性和产率分别为54.5%和27.1%。

    Abstract:

    Yttrium oxide, lanthanum oxide and cerium oxide modified SAPO-34 (M-SAPO-34,where M= Y 、La、Ce) were prepared by hydrothermal method, respectively. The samples were characterized by the methods of XRD, SEM, FT-IR, BET, NH3-TPD and TG. The results show that rare earths were added into SAPO-34 framework. They have higher specific surface area and smaller particles size, as well as the changes in the pore diameter and acidity. Bifunctional catalysts of CuO-ZnO-ZrO2/M-SAPO-34 were prepared by mechanically mixing M-SAPO-34 with CuO-ZnO-ZrO2 in the weight ratio of 1:1. Its catalytic activity for carbon dioxide hydrogenation to light olefins was investigated. Under the conditions of reaction temperature at 400℃, pressure at 3.0 MPa,space velocity (SV) of 1800 mL/(gcat •h),CO2/H2 (molar ratio) of 1:3,bifunctional catalyst mass of 1.0g, CuO-ZnO-ZrO2/La-SAPO-34 exhibited better catalytic activity, the conversion of CO2 could reach to 49.7% with a light olefins selectivity and yield of 54.5% and 27.1%, respectively.

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刘蓉,王鹏飞,査飞,田海峰,常玥.稀土改性SAPO-34分子筛的制备及其在CO2加氢合成低碳烯烃中的催化性能[J].精细化工,2016,33(4):

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  • 收稿日期:2015-12-24
  • 最后修改日期:2016-01-28
  • 录用日期:2016-02-17
  • 在线发布日期: 2016-03-10
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