CIESC Journal ›› 2018, Vol. 69 ›› Issue (7): 3009-3017.DOI: 10.11949/j.issn.0438-1157.20171428

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Effects of silylation and organic weak alkali modified Mo/HZSM-5 on catalytic performance in non-oxidative aromatization of methane reaction

TIAN Haifeng1,2, YAO Lu1, GAO Jialiang2, ZHA Fei1, GUO Xiaojun1   

  1. 1 College of Chemistry & Chemical Engineering, Northwest Normal University, Lanzhou 730070, Gansu, China;
    2 College of Chemical Engineering, Northwest University, Xi'an 710069, Shaanxi, China
  • Received:2017-10-26 Revised:2018-03-10 Online:2018-07-05 Published:2018-07-05
  • Supported by:

    supported by the Young Teacher Research Group Foundation of Northwest Normal University (NWNU-LKQN-16-6).

硅烷化和有机弱碱改性Mo/HZSM-5对甲烷无氧芳构化催化性能的影响

田海锋1,2, 姚璐1, 高佳良2, 查飞1, 郭效军1   

  1. 1 西北师范大学化学化工学院, 甘肃 兰州 730070;
    2 西北大学化工学院, 陕西 西安 710069
  • 通讯作者: 査飞
  • 基金资助:

    西北师范大学青年教师提升计划项目(NWNU-LKQN-16-6)。

Abstract:

The morphology of catalysts and the assembly of catalysts particles have important influence on the catalytic performance. The core-shell composite materials with Mo/HZSM-5 as the core and silicalite-1 zeolite as shell were prepared by silylation. The hollow structure of Mo/HZSM-5 catalyst microspheres with rich silicon surface and hierarchical pore structure was prepared by the weak organic alkali etching method. The structure of Mo/HZSM-5 were characterized by XRD, TEM, N2-adsorption-desorption and NH3-TPD. The surface acidity of Mo/HZSM-5 catalysts was modulated by silylation or the weak organic alkali etching method. The crystallinity, mesoporous specific surface and pore volume of Mo/HZSM-5 catalyst increased by the weak organic alkali etching method. The catalytic performance of Mo/HZSM-5 catalysts via different post-treatment was investigated, the results show that the catalyst stability could be improved and the distribution of the product has a significant influence in non-oxidative aromatization of methane reaction.

Key words: catalyst, chemical reaction, molecular sieves, methane, morphological structure

摘要:

催化剂的形态及晶粒的组装对其催化性能有重要影响,采用硅烷化处理对Mo基催化剂表面酸性进行毒化制备了核壳型(Mo基催化剂@Silicalite-1)复合材料;采用四丙基氢氧化铵或正丁胺有机弱碱对Mo/HZSM-5进行刻蚀,然后经过脱硅再结晶分别制备了表面富硅型中空结构Mo/HZSM-5微球和表面富硅、核内含有多级孔道的Mo/HZSM-5微球。采用XRD、TEM、N2等温吸脱附和NH3-TPD对催化剂结构进行表征,并考察了三种不同后处理方法对Mo基催化剂在甲烷无氧芳构化反应中催化性能的影响。硅烷化和有机碱处理均能够调变Mo/HZSM-5催化剂的表面酸性,而经有机碱处理以后,催化剂结晶度、介孔比表面积和孔容均具有不同程度的增加,三种不同后处理方法均能改善Mo/HZSM-5催化剂的反应稳定性,对产物的分布也产生了显著影响。

关键词: 催化剂, 化学反应, 分子筛, 甲烷, 形貌结构

CLC Number: