ITQ-24分子筛的合成及催化性能研究

石油炼制与化工 ›› 2021, Vol. 52 ›› Issue (10): 118-125.

ITQ-24分子筛的合成及催化性能研究

梁俊¹,²,汪莹莹²,李相呈²,刘闯²,沈少春²,付文华²,王振东²,杨为民^1,2

1. 华东理工大学化工学院
2. 中国石化上海石油化工研究院绿色化工与工业催化国家重点实验室

收稿日期:2021-05-31 修回日期:2021-06-17 出版日期:2021-10-12 发布日期:2021-09-29
通讯作者: 王振东 E-mail:wangzd.sshy@sinopec.com
基金资助:
国家重点研发计划项目;国家自然科学基金委员会面上项目

SYNTHESIS AND CATALYTIC PERFORMANCE OF ITQ-24 ZEOLITE

Received:2021-05-31 Revised:2021-06-17 Online:2021-10-12 Published:2021-09-29

摘要/Abstract

摘要： 以1,1’-[1,4-苯双亚甲基]双[1-甲基吡咯烷]氢氧化物为有机结构导向剂（OSDA）制备了ITQ-24分子筛，系统考察了GeO₂含量、OSDA用量、HF含量、晶化温度、搅拌速率对ITQ-24分子筛晶化的影响。并采用X-射线衍射（XRD）、扫描电子显微镜（SEM）、氨程序升温脱附（NH₃-TPD）和吡啶吸附红外光谱（Py-IR）等方法对晶化产物进行了表征。结果表明：适合ITQ-24分子筛晶化的初始凝胶组成为n（SiO₂）∶n（GeO₂）∶n（OSDA）∶n（H₂O）＝1∶（0.2～0.5）∶0.3∶（5～20），晶化条件为动态、170 ℃；所制得的ITQ-24分子筛具有较高的水热稳定性，含有较多的弱酸和Lewis酸位。将该分子筛应用于环己酮氧化制备ε-己内酯反应中，在80 ℃最佳反应温度下，环己酮的转化率为22.5%，ε-己内酯的选择性可达到54.5%。

关键词: ITQ-24, 分子筛, B-V氧化反应, 环己酮, ε-己内酯

Abstract: ITQ-24 zeolite was synthesized using 1,1’-[1,4-phenylenebis（methylene）] bis [1-methyl pyrrolidinium] hydroxide as organic structure-directing agent（OSDA）. The effects of Ge content，OSDA amount，HF content，crystallization temperature，and stirring speed on the crystallization of ITQ-24 zeolite were investigated,respectively. X-ray diffraction（XRD），scanning electron microscope（SEM），temperature-programmed desorption of NH₃（NH₃-TPD）and Fourier transform infrared spectroscopy of pyridine adsorption（Py-IR）methods were carried out to characterize the obtained zeolites. The suitable molar compositionn（SiO₂）∶n（GeO₂）∶n（OSDA）∶n（H₂O）for the crystallization of ITQ-24 zeolite is 1∶（0.2-0.5）∶0.3∶（5-20），and the optimum temperature is 170 ℃ under dynamic condition. The ITQ-24 zeolite has high hydrothermal stability and contains lots of weak and Lewis acid sites. In the oxidation reaction of cyclohexanone to ε-caprolactone，using ITQ-24 as catalyst,the ε-caprolactone selectivity reached 54.5% with 22.5% cyclohexanone conversion under the optimum temperature of 80 ℃.

Key words: ITQ-24, zeolite, Baeyer-Villiger oxidation, cyclohexanone, ε-caprolactone

梁俊汪莹莹李相呈刘闯沈少春付文华王振东杨为民. ITQ-24分子筛的合成及催化性能研究[J]. 石油炼制与化工, 2021, 52(10): 118-125.

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