纳米Ga-ZSM-5分子筛的合成及其在苯和稀乙烯烷基化反应中的应用
收稿日期: 2021-04-17
网络出版日期: 2022-03-14
基金资助
国家自然科学基金青年项目(22008019)
Synthesis of nano Ga-ZSM-5 zeolite and its application in alkylation of benzene with dilute ethylene
Received date: 2021-04-17
Online published: 2022-03-14
采用晶种导向法合成了一系列不同硅镓比的纳米级Ga-ZSM-5分子筛,经过挤条成型、酸洗以及高温焙烧等处理后得到了纳米Ga-ZSM-5分子筛催化剂。利用多种表征技术对Ga-ZSM-5分子筛的结构和酸性质进行了表征,研究了其催化苯与稀乙烯烷基化反应性能。结果表明,水热合成的Ga-ZSM-5分子筛具有十字孪晶状形貌,晶粒尺寸均匀。与相同n（Si）/n（T）（T为金属原子）的Al-ZSM-5分子筛相比,Ga-ZSM-5分子筛的酸量和酸强度明显降低。在反应温度为360 ℃、压力为1.4 MPa、乙烯质量空速（WHSV）为1.5 h-1、n（苯）∶n（乙烯）=1∶1,n（乙烯）∶n（氮气）=1∶5.67的反应条件下,Ga-ZSM-5分子筛催化剂表现出了较高的乙基选择性,副产物二甲苯比Al-ZSM-5减少了30%~50%,且在100 h内稳定运转,具有更好的抗积炭能力。
谢卓涵 , 韩贺 , 李孝国 , 张永坤 , 侯章贵 , 边凯 , 张安峰 , 郭新闻 , 宋春山 . 纳米Ga-ZSM-5分子筛的合成及其在苯和稀乙烯烷基化反应中的应用[J]. 无机盐工业, 2022 , 54(2) : 123 -128 . DOI: 10.19964/j.issn.1006-4990.2021-0251
A series of nano Ga-ZSM-5 zeolites with different Si/Ga ratio were synthesized with seed-oriented method.Ga-ZSM-5 catalysts were obtained with extrusion molding,acid pickling and high temperature roasting.The structure and acid properties of Ga-ZSM-5 zeolites were characterized by various techniques and their catalytic performance in the alkylation of benzene with dilute ethylene were evaluated.The results showed that hydrothermal synthesized Ga-ZSM-5 molecular sieves exhibited intergrown morphologies and uniform particle size.Compared with Al-ZSM-5 zeolites with the same n（Si）/n（T）（T was metal atom）,the acid content and acid strength of Ga-ZSM-5 zeolites were significantly reduced.Under the reaction conditions of T=360 ℃,P=1.4 MPa,weight hourly space velocity（WHSV） of ethylene=1.5 h-1,n（benzene）∶n（ethylene）=1∶1,n（ethylene）∶n（nitrogen）=1∶5.67,Ga-ZSM-5 zeolites catalysts showed higher ethylbenzene selectivity and 30%~50% reduction for xylene selectivity compared with Al-ZSM-5.In addition,Ga-ZSM-5 zeolites catalyst remained stable during the time on stream of 100 h with stronger coke-resistant capacity.
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