多级孔ZSM-5分子筛的一步合成及反应性能  

Synthesis of hierarchical ZSM-5 zeolite in dense system by one step and its catalytic property in MTP reaction

作　　者：张洪菡 张善鹤 李春义[1] ZHANG Hong - han;ZHANG Shan- he;LI Chun - yi(State Key Laboratory of Heavy Oil Processing, China University of Petroleum （ East China） , Qingdao 266580, Chin)

机构地区：[1]中国石油大学(华东)重质油国家重点实验室,山东青岛266580

出　　处：《石化技术与应用》2017年第6期429-433,共5页Petrochemical Technology & Application

基　　金：国家重点基础研究发展规划973计划资助项目(项目编号:2012 CB 215006)

摘　　要：采用水热晶化法,通过改变水量来调节初始凝胶浓度,在Na2O∶H2O∶四丙基溴化铵∶Si O2摩尔比为0.07∶x∶0.05∶1.00(x分别为5.00,15.00,25.00,35.00,对应的试样依次命名为试样1~试样4)下,合成了一系列多级孔ZSM-5分子筛。以此为基质,制备了用于甲醇转化制丙烯(MTP)反应的HZSM-5分子筛催化剂,并在连续流动固定床微反装置上,于甲醇空速为9.78 h-1,反应温度为450℃,反应时间为120 min及常压条件下,考察了分子筛催化剂的活性。结果表明:体系水量的改变对ZSM-5分子筛的骨架结构无明显影响;与传统微孔ZSM-5分子筛催化剂(试样4)相比,多级孔分子筛催化剂(试样1~试样3)因具有较好的传质特性和较大的比表面积,提高了催化剂活性、稳定性及丙烯收率;在多级孔分子筛催化剂(以试样2为基质)运行120 min内,转化率、丙烯收率和丙烯/乙烯(质量比)基本不变,依次约为100%,32%,7.5。A series of hierarchical ZSM - 5 zeo- lites were synthesized by traditional hydrothermal crystallization method and changing water content for regulating the concentration of initial gel at the mole ratio of Na20： H20：TPABr： SiO2 of 0.07：x：0. 05：1.00 （x = 5, 15, 25, 35, the samples were according named as sample 1 to sample 4）. The as - synthe- sized ZSM -5 zeolites were used as base to prepare acid HZSM -5 zeolite catalysts. Methanol to propyl- ene（MTP） catalysis properties were evaluated in a continuous flow fixed - bed microreactor under the conditions of atmospheric pressure, reaction tempera- ture 450 ~C , reaction time 120 min, volume space velocity 9. 78 h-l. The results showed that thechange of water content had no obvious effect on skeleton structure of ZSM -5. Compared with tradi- tional microporous ZSM - 5 zeolite （ sample 4）, hier- archical ZSM - 5 zeolite （ sample 1 - sample 3 ） with the better mass transfer property and the bigger sur- face area enhanced the activity stability of catalysts and the propylene yield. When hierarchical ZSM -5 zeolite based catalysts （sample 2 as the matrix）had been running for 120 min,the methanol conversion propylene yield and propylene/ethylene（ mass ratio was 100% ,32% and 7.5 in turn.

关 键 词：多级孔 ZSM-5分子筛 催化剂 甲醇 丙烯 转化率 

分 类 号：TQ223.121[化学工程—有机化工]