CIESC Journal ›› 2015, Vol. 66 ›› Issue (9): 3470-3475.DOI: 10.11949/j.issn.0438-1157.20150849

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Isopropylation of 4-isopropybiphenyl to 4,4'-diisopropylbiphenyl over alkalis and acid modified mordenite zeolites

LIU Min1, SHEN Zhongming1, GUO Xinwen1, SONG Chunshan1,2   

  1. 1 PSU-DUT Joint Center for Energy Research, State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China;
    2 EMS Energy Institute, Department of Energy & Mineral Engineering, Pennyslvania State University, Pennyslvania 16802, United States
  • Received:2015-06-08 Revised:2015-06-15 Online:2015-09-05 Published:2015-09-05

酸碱复合改性丝光沸石催化4-异丙基联苯异丙基化

刘民1, 沈忠明1, 郭新闻1, 宋春山1,2   

  1. 1 大连理工大学化工学院, 精细化工国家重点实验室, 宾州-大连联合能源研究中心, 辽宁 大连 116024;
    2 宾州州立大学能源研究所, 能源与矿物工程系, 美国 宾夕法尼亚 16802
  • 通讯作者: 郭新闻

Abstract:

Isopropylation of 4-isopropybiphenyl to 4,4'-diisopropylbiphenyl was carried out over hierarchical mesoporousmordenite zeolites through alkalis modification of H-mordenite zeolite in a fixed-bed reactor. In order to investigate the effects of the pore structure and the acid sites of the zeolite samples on the catalytic properties, the parent and modified zeolite samples were thoroughly characterized with X-ray diffraction (XRD), transmission electron microscopy (TEM), ammonia temperature programmed desorption (NH3-TPD), and N2 physical adsorption-desorption. The results showed that the alkalis treatment adapted the pore structure, and the acid strength and amount without obvious destruction to the MOR topological structure. This adaption was contributed to the improvements of 4-isopropybiphenyl conversion and reaction stability. Modifying the sample with alkalis first and then followed by an acid treatment was in favor of removing the extra-framework alumina from the alkalis treatment and adapting the acid sites on the extra surface of the sample, which can successfully improve the selectivity of 4,4'-diisopropylbiphenyl.

Key words: H-mordenite, hierarchical mesoporous, 4-isopropybiphenyl, 4,4'-diisopropylbiphenyl, alkylation, catalysis, selectivity, preparation

摘要:

采用酸碱复合改性的方法,制备了同时具有微孔和介孔孔道的丝光沸石,用于固定床4-异丙基联苯的异丙基化反应。通过X射线衍射(XRD)、透射电子显微镜(TEM)、NH3程序升温脱附(NH3-TPD)、N2物理吸附脱附等方法对改性丝光沸石进行表征。结果表明,碱改性处理调变了丝光沸石的孔道结构和酸性质,同时保持了其MOR拓扑结构,提高了4-异丙基联苯的转化率和反应的稳定性。碱处理后再进行酸处理,可以有效清除碱处理过程中产生的非骨架铝物种和样品外表面的酸中心,提高目的产物4,4'-二异丙基联苯的选择性。

关键词: 丝光沸石, 多级孔, 4-异丙基联苯, 4,4'-二异丙基联苯, 烷基化, 催化, 选择性, 制备

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