复合金属改性镁碱沸石在合成气制二甲醚中的应用  

Application of Ferrierite Modified by Composite Metal in Direct Synthesis of Dimethyl Ether from Syngas

作　　者：张海燕[1] 郝治富[1] 吴玮[1] 宁英男[1] 毛国梁[1] 

机构地区：[1]东北石油大学化学化工学院石油与天然气化工省重点实验室,黑龙江大庆163318

出　　处：《化学反应工程与工艺》2011年第2期133-138,共6页Chemical Reaction Engineering and Technology

基　　金：大庆市科学技术计划项目(SGG2007-39)

摘　　要：采用浸渍法对镁碱沸石(FER)进行了Zn-Mn复合金属改性,将改性后的FER作为合成气直接制二甲醚催化剂的甲醇脱水组分,制备出了Cu-Zn-Al/FER-Zn-Mn双功能催化剂。在连续固定床高压反应器中,考察了改性条件对催化剂性能的影响。采用吡啶吸附红外光谱(Py-IR)和X射线衍射(XRD)对改性前后的催化剂进行表征,并测定了催化剂的比表面积、孔体积及孔径。结果表明,当Zn(NO_3)_2质量分数为4%,Mn(NO_3)_2质量分数为3%,改性浸渍时间3.5 h,浸渍温度80℃和焙烧温度450℃时,Cu-Zn-Al/FER-Zn-Mn催化剂的催化效果较好,在反应温度260℃、反应压力3.2 MPa、空速1500 h^(-1)和H_2与CO物质的量之比为2的条件下,CO的转化率为83.0%,二甲醚选择性为73.0%,催化剂性能优于改性前的FER。Ferrierite（FER） was modified by Zn-Mn composite metal through dipcoating method and the modified FER was used as the dehydrating agent to prepare Cu-Zn-AI/FER-Zn-Mn bifunctional catalyst for the direct synthesis of dimethyl ether from syngas. Effects of modification conditions on the performance of the catalysts were investigated in a continuous fixed-bed reactor. The catalysts were characterized by means of pyridine adsorption infrared spectroscopy（Py-lR） and X-ray diffraction（XRD）. The Cu-Zn-AI/FER-Zn-Mn catalyst that was treated by mass fraction 4% Zn（NO3）2 solution and mass fraction 3% Mn（NO3）2 solution for 3.5 h at 80℃ and caleinated at 450 ℃ exhibited excellent catalytic performance. The conversion of CO and selectivity of dimethyl ether reached 83.0% and 73.0%, respectively, under the conditions of reaction temperature 260 ℃, reaction pressure 3.2 MPa, space velocity 1 500 h^-l and molar ratio of H2 to CO 2. The catalytic performance of the modified FER catalysts was better than that of the catalysts made from unmodified FER.

关 键 词：合成气 二甲醚 镁碱沸石 硝酸锌 硝酸锰 浸渍法 金属改性 

分 类 号：TQ426[化学工程] TQ223.2