纳米薄层HZSM-5分子筛催化甲醇制丙烯  

Methanol to Propylene over Nanosheets of HZSM-5 Zeolite

作　　者：张少龙 张兰兰 王务刚 闵媛媛 马通 宋宇 巩雁军 窦涛[1] 

机构地区：[1]中国石油大学(北京)化学工程学院,重质油国家重点实验室,中国石油天然气集团公司催化重点实验室,北京102249

出　　处：《物理化学学报》2014年第3期535-543,共9页Acta Physico-Chimica Sinica

基　　金：国家重点基础研究发展规划项目(973)(2012CB215002);国家自然科学基金(21276278;21176255);中国石油股份公司(2011A-2101)资助~~

摘　　要：在合成系列硅铝比纳米薄层HZSM-5分子筛的基础上,研究了纳米薄层HZSM-5分子筛催化甲醇制丙烯(MTP)的反应性能.在固定床微反装置上详细考察了工艺条件对纳米薄层HZSM-5分子筛催化性能的影响,同时与纳米HZSM-5分子筛对MTP反应的催化性能进行了比较.结果表明,纳米薄层HZSM-5分子筛具有较高的目的产物选择性和较长的催化寿命.在适宜硅铝比(n(SiO2)/n(Al2O3)=213)和反应条件下(温度470°C,甲醇质量空速为3 h-1),丙烯的选择性达到46.7%,三烯(乙烯、丙烯和C4烯烃)选择性达到78.7%.其中,丙烯/乙烯的质量比可达到6.5,是纳米HZSM-5分子筛的2倍,而芳烃的选择性比纳米分子筛明显降低.这是因为纳米薄层HZSM-5分子筛比纳米HZSM-5分子筛具有较宽的(010)晶面、较大的外比表面积和介孔孔容.Nanosheets of HZSM-5 zeolite with different SiO2/Al2O3 molar ratios were synthesized, and their catalytic behavior in the methanol-to-propylene （MTP） reaction was evaluated in a fixed bed reactor. The effect of reaction conditions on catalytic performance was studied in detail. The catalytic performance of nanosheets of HZSM-5 zeolites in the MTP reaction was compared with that of the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite had higher propylene selectivity, total three olefins′selectivity （ethylene, propylene, C4 alkenes）, and a longer catalytic lifetime than the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite with a SiO2/Al2O3 molar ratio of 213 yielded a propylene selectivity of 46.7%, total three olefins′selectivity of 78.7%at 470 ＆#176;C, and a methanol weight hourly space velocity （WHSV） of 3 h-1. It also yielded a propylene/ethylene mass ratio of 6.5, which was double that of the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite had a lower aromatic selectivity than the nanosized HZSM-5 zeolite. The good MTP catalytic performance of the nanosheets of HZSM-5 zeolite was attributed to their wide （010） surface, high external surface area, and large mesoporous volume.

关 键 词：纳米薄层 HZSM-5分子筛 甲醇 丙烯 

分 类 号：TQ221.212[化学工程—有机化工]