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改性Hβ沸石分子筛的制备及烷基化性能
作者:    陈政利     杨丽娜   
单位:(辽宁石油化工大学石油化工学院 辽宁 抚顺 113001) 
关键词:氢型β分子筛 烷基化 二苯甲烷 多级孔 Lewis酸 改性 
分类号:TQ426.94
出版年,卷(期):页码:2019,47(6):0-0
DOI:
摘要:

 采用碱处理Hβ沸石得到含介孔结构的Hβ分子筛,再使用浸渍法制备了Fe-多级孔Hβ催化剂。通过X射线荧光光谱仪,X射线衍射仪,N2吸附–脱附等温曲线,扫描电子显微镜,吡啶吸附-Fourier红外光谱仪,热重分析对样品进行表征。结果表明:NaOH处理Hβ后成功引入介孔,Fe改性并未破坏载体结构。碱处理扩大了Hβ孔径,有效的提高了反应物和产物的扩散性能;Fe改性增加了催化剂表面活性中心数量,提高了催化剂表面Lewis酸含量。考察了碱处理浓度、时间,焙烧温度、时间对烷基化性能的影响。在碱处理浓度0.1 mol/L,碱处理时间30 min,焙烧温度450 ℃,焙烧时间4 h的最佳制备条件下,制备出的Fe-多级孔Hβ催化剂的氯苄转化率为99.7%,二苯甲烷的选择性达到81.2%。

  The mesoporous molecular sieve was obtained via alkali treatment with Hβ zeolite molecular sieve, and Fe-hierarchical porous Hβ catalyst was prepared by an impregnation method. The samples were characterized by X-ray fluorescence spectroscopy, X-ray diffraction, N2 adsorption–desorption isothermal analysis, scanning electronic microscopy, pyridine Fourier transform infrared spectroscopy, and thermogravimetric analysis. The results show that treatment of NaOH introduces mesopores, and the introduction of Fe does not destroy the carrier structure. Alkali treatment increases the pore size of Hβ and effectively improves the diffusion properties of reactants and products. Fe modification increases the number of surface active sites of the catalyst and increases the Lewis acid content on the surface of the catalyst. The effects of alkali treatment concentration, alkali treatment time, calcination temperature and calcination time on the alkylation performance were investigated. The benzyl chloride conversion rate of Fe-hierarchical porous Hβ catalyst prepared under the optimal conditions (i.e., alkali treatment concentration of 0.1 mol/L, alkali treatment time of 30 min, calcination temperature of 450 ℃ and calcination time of 4 h) is 99.7%, and the selectivity of diphenylmethane reaches 81.2%.

基金项目:
国家自然科学基金(21276120);辽宁省高等学校杰出青年学者成长计划(LJQ2015062);辽宁省科学技术厅项目(20170540585)。
作者简介:
参考文献:

 [1] 詹金友, 张耀兵, 张璐璐, 等. SbCl3/SBA-15的制备及催化合成二苯甲烷性能[J]. 石油学报(石油加工), 2016, 32(4): 780–786. 

ZHAN Jinyou, ZHANG Yaobing, ZHANG Lulu, et al. J Pet (Pet Process) (in Chinese), 2016, 32(4): 780–786. 
[2] 刘森, 杜耘辰, 肖霓, 等. 一锅法合成介孔材料Fe-SBA-15及其对Friedel-Crafts苄基化反应的催化性能[J]. 催化学报, 2008, 29(5): 468–472. 
LIU Sen, DU Yunchen, XIAO Ni, et al. Chin J Catal (in Chinese), 2008, 29(5): 468–472. 
[3] 纪敏, 吴海鸣, 贺民, 等. 固载化AlCl3催化合成二苯基甲烷反应动力学研究[J]. 大连理工大学学报, 2008, 48(2): 168–172. 
JI Min, WU Haiwei, HE Min, et al. J Dalian Univ Technol (in Chinese), 2008, 48(2): 168–172. 
[4] 周春辉, 罗锡平, 葛忠华, 等. 酸化粘土负载ZnCl2催化剂的制备及其对苯苄基化反应的催化性能[J]. 催化学报, 2003, 24(8): 579–584. 
ZHOU Chunhui, LUO Xiping, GE Zhonghua, et al. Chin J Catal (in Chinese), 2003, 24(8): 579–584. 
[5] 杨菊红, 韩晓祥, 陈青, 等. 离子液体催化苯与苄氯的烷基化合成二苯甲烷[J]. 精细化工, 2010, 27(6): 610–613. 
YANG Juhong, HAN Xiaoxiang, CHEN Qing, et al. Fine Chem (in Chinese), 2010, 27(6): 610–613. 
[6] 秦涛, 毕亚东, 雷晓娟, 等. NaOH后处理对多级孔Hβ分子筛上木质素催化热解性能的影响[J]. 燃料化学学报, 2018, 46(9): 1074–1078. 
QIN Tao, BI Yadong, LEI Xiaojuan, et al. J Fuel Chem Technol (in Chinese), 2018, 46(9): 1074–1078. 
[7] 王海彦, 宋盼盼, 王钰佳. 多级孔Hβ沸石对NiWP/Hβ-Al2O3催化剂柴油加氢性能的影响[J]. 燃料化学学报, 2016, 44(4): 470–476. 
WANG Haiyan, SONG Panpan, WANG Yujia. J Fuel Chem Technol (in Chinese), 2016, 44(4): 470–476. 
[8] 郭永乐, 张钰, 赵忠奎. 氧化铈改性多级孔Hβ分子筛催化对二甲苯与苯乙炔烯基化反应(英文)[J]. 催化学报, 2018, 39(1): 181–189. 
GUO Yongle, ZHANG Yu, ZHAO Zhongkui. Chin J Catal, 2018, 39(1): 181–189. 
[9] BI Y, LEI X, XU G, et al. Catalytic fast pyrolysis of kraft lignin over hierarchical HZSM-5 and Hβ zeolites[J]. Catalysts, 2018, 8(2): 82–95. 
[10] XIONG Y, CHEN W, ZENG A. Optimization for catalytic performances of Hβ zeolite in the acylation of 2-methylfuran by surface modification and solvents effect[J]. Res Chem Intermed, 2017, 43(3): 1557–1574. 
[11] KHAN A, CHEN P, BOOLCHAND P, et al. Modi?ed nano-crystalline ferrites for high-temperature WGS membrane reactor applications[J]. J Catal, 2008, 253(1): 91–104. 
[12] 范峰, 凌凤香, 王少军, 等. 核壳结构的Beta-Y复合分子筛的合成与表征[J]. 燃料化学学报, 2012, 40(7): 861–865. 
FAN Feng, LING Fengxiang, WANG Shaojun, et al. J Fuel Chem Technol (in Chinese), 2012, 40(7): 861–865. 
[13] LIU J, CUI L, WANG L, et al. Alkaline-acid treated mordenite and beta zeolites featuring mesoporous dimensional uniformity[J]. Mater Lett, 2014, 132(10): 78–81. 
[14] 王俊丰, 沈健, 石薇薇. Ce/USY改性分子筛催化苯酚甲醇烷基化的实验研究[J]. 石油学报(石油加工), 2017, 33(4): 757-762. 
WANG Junfeng, SHEN Jian, SHI Weiwei. J Pet (Pet Process) (in Chinese), 2017, 33(4): 757–762. 
[15] 项寿鹤, 王敬中, 高峰, 等. Hβ沸石上L酸的研究[J]. 催化学报, 1991, 12(5): 404–408. 
XIANG Shouhe, WANG Jingzhong, GAO Feng, et al. Chin J Catal (in Chinese), 1991, 12(5): 404–408. 
[16] 杨勇, 陶智超, 张成华, 等. 焙烧温度对Fe-Mn催化剂结构和F-T合成性能影响[J]. 燃料化学学报, 2004, 32(6): 717–722. 
YANG Yong, TAO Zhichao, ZHANG Chenghua, et al. J Fuel Chem Technol (in Chinese), 2004(6): 717–722. 
[17] CHUABE V D. Benzylation of benzene to diphenyl methane using zeolite catalysts[J]. Catal Commun, 2004, 5(6): 321–326.
 
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