cufehzsm催化剂的改性及其协同等离子体活化co2加氢合成二甲醚的研究.docx

优秀毕业论文 精品参考文献资料 Cu． Cu．Fe／HZSM．5催化剂在1 5 h内保持稳定。 其次，采用均匀沉淀法制备了一系列不同Ce02含量的Cu-Fe—Ce催化剂， 将其与HZSM-5催化剂机械混合后以C02加氢合成二甲醚为探针反应考察 催化剂的活性和稳定性。Ce02改性Cu．Fe催化剂形成了稳定的固溶体，促 进了CuO的分散，减小了CuO的晶粒尺寸，降低了高分散CuO的还原温 度，改变了Cu．Fe．Ce催化剂的比表面积。同时，Ce02加入Cu-Fe催化剂能 够改变酸量和酸类型，促使C02加氢合成二甲醚的催化性能提高。在 Z(H2)／V(C02)为4，260。C、3．0 MPa、1500 mL·goat1．h。1的条件下，将Ce02 含量为3 wt％的Cu-Fe．Ce／HZSM．5催化剂用于C02加氢合成二甲醚反应， C02转化率、二甲醚选择性分别达到20．9％、63．1％。 再次，在C02进入固定床反应器前，通过高压放电等离子体使C02活 化后再在Ce02含量为3．0 wt％的Cu-Fe．Ce／HZSM．5上进行C02加氢合成二 甲醚反应，并研究了该过程的本征动力学。与单独使用Cu．Fe．Ce／HZSM一5 催化剂相比，等离子体活化结合加氢过程时，C02转化率、二甲醚选择性分 别提高了16．3％、10．1％，说明等离子体活化作用提高了C02的反应性能。 本征动力学研究发现，甲醇合成反应、逆水煤气反应、甲醇脱水生成二甲醚 反应的活化能分别为149．34 kJ．mol～、75．47 kJ．mol～、73．18 kJ·mol～，比单 独使用Cu—Fe．Ce／HZSM．5催化剂时的活化能分别低了13．05 kJ·mol～、46．20 kJ．mol～、13．33 kJ-mol～，表明等离子体活化能够降低催化反应的活化能来 提高C02加氢合成二甲醚的产率。 关键词：二氧化碳催化加氢二甲醚等离子体本征动力学 万方数据 THE THE STUDY OF THE MODIFICATION OF THE Cu．Fe／HZSM．5 AND ITS SYNERGIZE PLASMLA To ACTI、编TE C02 HYDROGENATION TO DIMETHYL ETHER ABSTRACT Dimethyl ether(DME)is a clean fuel，using as domestic fuel and power fuel alternative to liquefied petroleum gas and diesel fueL and it is also an．．important chemical intermediates，which exhibition a wide range of application prospects． C02 is a main greenhouse gas，and the C02 hydrogenation to DME is an important way to convert C02，which Can reduce the pollution of C02，and ease the energy shortage．However,C02 molecule was very stable，and the conversion of the C02 Was difficult．It is a innovation to study the efficient catalysts and use the C02 to react atter activation． In the present paper,the modification of the Cu-based catalysts for C02 hydrogenation to DME were studied，and the plasma is introduced to active the reactant．The following three aspects are studied： Firstly,Cu—Fe／HZSM一5 bifunctional catalysts were modified with La，Ce and were applied for the direct synthesis of DME from C02 and HE．The catalysts 。Supported by National Natural Science Foundation of China(2 1 366004，2 1 00603 1)，the Open Project of Guangxi Key La