脱铝超稳Y沸石负载磷钨酸铯盐催化合成乙二醇二甲醚  

Synthesis of dimethoxyethaneover cesium phosphotungstate supported on dealuminated ultra stable Y zeolite catalyst

作　　者：于清跃 张云良 孙飞 朱新宝[3] 

机构地区：[1]南京科技职业学院化工与材料学院,江苏南京210048 [2]南京安鼎化工科技有限公司,江苏南京210048 [3]南京林业大学化学工程学院,江苏南京210037

出　　处：《石油化工》2017年第11期1366-1372,共7页Petrochemical Technology

基　　金：江苏高校科研产业化项目(JHZD2012-15);江苏"青蓝工程"基金项目;江苏高校校长基金资助项目;骨干教师境外研修(2013)基金资助项目

摘　　要：采用水蒸气脱铝法制备脱铝超稳Y沸石(DUSY)载体,负载磷钨酸铯盐(Cs_(2.5)PW)制备了系列催化剂,并在固定床反应器上考察了系列催化剂催化二甲醚(DME)与环氧乙烷(EO)合成乙二醇二甲醚(DMEG)反应的性能,优化了Cs_(2.5)PW负载量、GHSV、反应温度、反应压力、催化剂的使用时间等条件。采用XRD、^(31)P NMR、^(29)Si NMR、N_2吸附-脱附、FTIR等方法对催化剂进行表征。表征结果显示,系列催化剂试样与DUSY载体发生了强相互作用,在DUSY表面高度分散且保持完整Y沸石的孔道结构。实验结果表明,在Cs_(2.5)PW负载量为30%(w)时,催化剂试样的NH_3吸附量可达618μmol/g,B酸与L酸吸附量分别为350,268μmol/g;在n(DME):n(EO)=3,80℃,GHSV=1 800 h^(-1),0.70 MPa,反应30 h的最优条件下,EO完全转化,DMEG选择性达62.6%;连续反应240 h后,EO转化率达98.1%,DMEG选择性未见下降,催化剂保持着较好活性。The catalyst for synthesis of dimethoxyethane（DMEG） with ethylene oxide（EO） and dimethyl ether（DME） on one-step way in fixed-bed is prepared by cesium phosphotungstate（Cs2.5PW） supported on ultra-stable Y zeolite water vapor dealumination. The catalyst is characterized by XRD, 31P NMR, 29Si NMR, N2 adsorption-desorption and FTIR. The result shows that cesium phosphotungstate takes a great interaction with dealuminium ultra stable Y zeolite（DUSY）. Cs2.5PW presents highly distribution on the supporter when the loading amount reaches 30%（w）. The N2 adsorption of catalyst reaches 618 μmol/g. When optimal conditions are mole ratio DME to EO of 3, reaction temperature 80 ℃, reaction pressure 0.70 MPa, and mixed gaseous hourly space velocity of 1 800 ha, the reaction shows that conversion of EO is 100.0%, and yield of dimethoxyethane 62.6%. When the catalyst continuous works 240 h, conversion of EO is 98.1% and selectivity of main product keeps no decreasing significantly.

关 键 词：环氧乙烷 二甲醚 乙二醇二甲醚 磷钨酸铯盐 

分 类 号：TQ426.6[化学工程]