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纳米薄层HZSM-5分子筛催化甲醇制丙烯
引用本文:张少龙,张兰兰,王务刚,闵媛媛,马通,宋宇,巩雁军,窦涛.纳米薄层HZSM-5分子筛催化甲醇制丙烯[J].物理化学学报,2014,30(3):535-543.
作者姓名:张少龙  张兰兰  王务刚  闵媛媛  马通  宋宇  巩雁军  窦涛
作者单位:State Key Laboratory of Heavy Oil Processing, The Key Laboratory of Catalysis, China National Petroleum Corporation, College of Chemistry Engineering, China University of Petroleum-Beijing, Beijing 102249, P. R. China
基金项目: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)及中国石油股份公司(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.

关 键 词:纳米薄层  HZSM-5分子筛  甲醇  丙烯  
收稿时间:2013-11-29
修稿时间:2014-01-03

Methanol to Propylene over Nanosheets of HZSM-5 Zeolite
ZHANG Shao-Long,ZHANG Lan-Lan,WANG Wu-Gang,MIN Yuan-Yuan,MATong,SONG Yu,GONG Yan-Jun,DOU Tao.Methanol to Propylene over Nanosheets of HZSM-5 Zeolite[J].Acta Physico-Chimica Sinica,2014,30(3):535-543.
Authors:ZHANG Shao-Long  ZHANG Lan-Lan  WANG Wu-Gang  MIN Yuan-Yuan  MATong  SONG Yu  GONG Yan-Jun  DOU Tao
Institution:State Key Laboratory of Heavy Oil Processing, The Key Laboratory of Catalysis, China National Petroleum Corporation, College of Chemistry Engineering, China University of Petroleum-Beijing, Beijing 102249, P. R. China
Abstract: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 ℃, 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.
Keywords:Nanosheet  HZSM-5 zeolite  Methanol  Propylene
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