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202106002.pdf
文章编号： 1672-6987（2021）06-0021-07； DOI： 10.16351/j.1672-6987.2021.06.002
张世忠a， 于凤丽a*， 王志萍b， 解从霞a(青岛科技大学 a.化学与分子工程学院；b.化工学院，山东 青岛 266042）
摘要： 通过碱处理对β沸石进行脱硅扩孔，制备成氢型后负载不同质量的三氟甲烷磺酸（TfOH），用于催化异丁烷与2-丁烯的烷基化反应。扩孔后Hβ沸石的微-介孔结构，有利于延长催化剂的使用寿命；TfOH的负载可以适当提高催化剂B/L酸性位点的比例，有利于提高烷基化产物的选择性。对改性后的催化剂进行了X射线荧光光谱分析、粉末X射线衍射、N2吸附脱附等温线、吡啶红外光谱、NH3-TPD等分析或表征。以固定床反应器，通过连续进样的方式探究了不同TfOH负载量的催化剂及反应条件对异丁烷/2-丁烯烷基化反应性能的影响。当TfOH的负载量占β沸石质量的20%，催化效果最佳。在反应温度80 ℃，反应压力2.5 MPa，烯烃质量空速0.8 h-1的优化条件下，催化剂有更长的寿命而且烯烃有较高的转化率，C8产物的选择性保持在65%以上。
关键词： 异丁烷； 2-丁烯； 烷基化； 三氟甲烷磺酸； β沸石； 脱硅
中图分类号： O 643； O 621文献标志码： A
引用格式： 张世忠， 于凤丽， 王志萍， 等. 微-介孔Hβ沸石负载三氟甲烷磺酸催化异丁烷/2-丁烯的烷基化反应［J］. 青岛科技大学学报(自然科学版), 2021, 42(6): 21-27.
ZHANG Shizhong， YU Fengli， WANG Zhiping，et al. Alkylation of isobutane/2-butene catalyzed by meso-microporous Hβ zeolites loaded with trifluoromethanesulfonic acid［J］. Journal of Qingdao University of Science and Technology（Natural Science Edition), 2021， 42（6）： 21-27.
Alkylation of Isobutane/2-Butene Catalyzed by Meso-microporous Hβ Zeolites
Loaded with Trifluoromethanesulfonic AcidZHANG Shizhonga， YU Fenglia， WANG Zhipingb， XIE Congxiaa
(a.College of Chemistry and Molecular Engineering; b.College of Chemical Engineering,
Qingdao University of Science and Technology, Qingdao 266042, China)
Abstract: By desilicating in alkaline solution, cation exchanging, and loading of trifluoromethanesulfonic acid (TfOH), meso-microporous Hβ zeolite catalyst was prepared and used to catalyze the alkylation of isobutane and cis-2-butene. After pore expansion, the hierarchical pore structure of Hβ zeolite is beneficial to prolong the lifetime of the catalyst; the loading of TfOH can appropriately increase the ratio of B/L acid sites in the catalyst, which is beneficial to increase the selectivity of alkylation products. The modified catalyst was analyzed or characterized by X-ray fluorescence spectroscopy, powder X-ray diffraction, N2 adsorption and desorption isotherm, pyridine infrared spectrum, and NH3-TPD. Using a fixed bed as a reactor, the effects of catalysts with different amounts of TfOH loading and reaction conditions on the catalytic performance of isobutane/2-butene alkylation were investigated by continuous sample injection. When the loading of TfOH accounts for 20% of the mass of β zeolite, the catalyst shows the best performance. Under the optimized conditions of reaction temperature of 80 ℃, reaction pressure of 2.5 MPa, and the weight hourly space velocity (WHSV) of 0.8 h-1, a high olefin conversion can be maintained for a long time, and the selectivity of C8 products can be maintained above 65%.
Key words: isobutane; 2-butene; alkylation; trifluoromethanesulfonic acid; β zeolite; desilication
收稿日期： 2020-12-24
基金项目： 国家自然科学基金项目（21805158，21476120）；山东省重点研发计划项目（2019GGX102021,2017GGX40107）.
作者简介： 张世忠（1995—），男，硕士研究生.*通信联系人.
