李春艳,张雅静,王康军,杜杰,王琦,吴静.尿素燃烧法制备CuO-ZnO/HZSM-5及其催化CO2加氢合成二甲醚的性能[J].分子催化,2017,31(4):365-371 |
尿素燃烧法制备CuO-ZnO/HZSM-5及其催化CO2加氢合成二甲醚的性能 |
Preparation of CuO-ZnO/HZSM-5 by Urea Combustion Method and Catalytic Property for Synthesis of Dimethyl Ether from CO2 Hydrogenation |
投稿时间:2017-05-23 修订日期:2017-06-26 |
DOI: |
中文关键词: 燃烧法 二甲醚 二氧化碳加氢 |
英文关键词:combustion dimethyl ether CO2 hydrogenation |
基金项目:国家自然科学基金项目(No.51301114,21203125),辽宁省高等学校优秀人才支持计划项目LNET(LJQ2013044),辽宁省自然科学基金(201602598,2015020649) |
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中文摘要: |
以尿素为燃烧剂,先采用燃烧法制备CuO-ZnO催化剂,接着采用研磨法将其与HZSM-5分子筛均匀混合形成CuO-ZnO/HZSM-5双功能催化剂.采用固定床反应器,在反应温度260℃、压力3.0 MPa、空速1 500 h-1条件下,考察了不同Cu/Zn(摩尔比)催化剂在CO2加氢合成二甲醚反应中的催化性能.通过XRD、N2等温吸附脱附、H2-TPR、NH3-TPD对催化剂进行表征,研究了不同Cu/Zn对催化剂结构及表面酸性的影响.结果表明:当Cu:Zn=6:4时,催化剂对CO2催化加氢直接合成二甲醚反应的催化活性和选择性最佳,CO2的转化率、DME的选择性分别为11.95%和28.74%,且在催化剂上具有更多的低温还原Cu和较强的酸中心,从而提高了CO2加氢活性和二甲醚的选择性. |
英文摘要: |
The CuO-ZnO catalyst were synthesized using urea as fuel by combustion method, then mixed with HZSM-5 zeolite by grinding method and form a bifunctional catalyst. The catalytic performance of catalyst with different Cu/Zn (molar ratio) for the synthesis of dimethyl ether from CO2 hydrogenation were tested, at reaction temperature 260℃, pressure of 3.0 MPa, space velocity 1 500 h-1 over a fixed-bed reactor. XRD, N2 isothermal adsorption-desorption, H2-TPR and NH3-TPD were employed to characterize the structure and surface properties of the catalysts with different Cu/Zn. The result indicated that the maximum catalytic activity and selectivity was obtained from the catalyst prepared when Cu:Zn was 6:4. The conversion of CO2 was 11.95%, the selectivity and the yield of dimethyl ether were 28.74% and 3.34% respectively. The catalyst with appropriate Cu/Zn showed better catalytic performance due to smaller grain size, better disperse of CuO species and suitable surface acidity. |
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