化工进展 ›› 2019, Vol. 38 ›› Issue (06): 2791-2795.DOI: 10.16085/j.issn.1000-6613.2018-1897

• 工业催化 • 上一篇    下一篇

超稳Y型分子筛的骨架硅铝比对甘油气相脱水反应的影响

韩琪1(),李海岩2,杨英1,刘百军1()   

  1. 1. 中国石油大学(北京)化学工程与环境学院重质油国家重点实验室,北京 102249
    2. 中国石油天然气股份有限公司大庆化工研究中心,黑龙江 大庆 163714
  • 收稿日期:2018-09-20 出版日期:2019-06-05 发布日期:2019-06-05
  • 通讯作者: 刘百军
  • 作者简介:韩琪(1989—),女,博士研究生,研究方向为催化剂及催化新材料。E-mail:<email>hq_8933@163.com</email>。

Influence of the SiO2/Al2O3 ratio on the performance of USY zeolites for the gas-phase dehydration of glycerol to acrolein

Qi HAN1(),Haiyan LI2,Ying YANG1,Baijun LIU1()   

  1. 1. State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering and Environment,China University of Petroleum,Beijing 102249,China
    2. Daqing Chemical Research Center of PetroChina,Daqing 163714,Heilongjiang, China
  • Received:2018-09-20 Online:2019-06-05 Published:2019-06-05
  • Contact: Baijun LIU

摘要:

以铵交换和高温水热处理法制备了不同硅铝比的超稳Y型分子筛(USY),利用X射线衍射、扫描电镜、氮气吸附脱附和吡啶红外等技术对USY进行了表征。以USY为催化剂,考察了USY的骨架硅铝比对气相甘油脱水制丙烯醛的影响。X射线衍射和扫描电镜结果表明,铵交换和高温水热处理只是提高USY的硅铝比,相对结晶度略有降低,而对Y型分子筛的结构和形貌没有影响。氮气吸附-脱附和吡啶红外结果表明,随USY骨架SiO2/Al2O3比提高,总酸量和B酸酸量逐渐降低,L酸酸量有所增多,介孔孔体积和平均孔径有所增大。气相甘油脱水反应结果表明,催化剂织构性质对甘油转化率和丙烯醛选择性的影响大于酸性的影响,因而SiO2/Al2O3比为29的USY催化剂的反应性能最好,甘油转化率和丙烯醛收率分别达到了84.5%和51.8%。

关键词: 超稳Y型分子筛, 骨架硅铝比, 催化, 甘油, 丙烯醛

Abstract:

The USY zeolites with different SiO2/Al2O3 ratios were prepared from commercial USY zeolites via the ammonium exchange and hydrothermal treatment and then were characterized by XRD, SEM, N2 adsorption and desorption isotherms and py-IR. The influence of SiO2/Al2O3 ratio on the performance of USY zeolites for the gas-phase dehydration of glycerol to acrolein was investigated. The results of XRD and SEM showed that the ammonium exchange and hydrothermal treatment only increased the SiO2/Al2O3 ratio and decreased the relative crystallinity of USY but had no effect on the structure and morphology of USY. The analysis of N2 adsorption and desorption isotherms and py-IR demonstrated that the total and B acid content of the USY gradually decreased, L acid content, mesoporous volume and mean pore size increased with the increase of framework SiO2/Al2O3 ratio. Activity evaluation results revealed that the textural property had more important effect on glycerol conversion and acrolein selectivity than the acid property. Therefore, USY with a SiO2/Al2O3 ratio of 29 displayed the best catalytic performance, giving an acrolein yield of 51.8% and glycerol conversion of 84.5%.

Key words: USY zeolite, framework SiO2/Al2O3 ratio, catalysis, glycerol, acrolein

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