Synthesis, characterization and catalytic performance of SAPO-34 molecular sieves for methanol-to-olefin (MTO) reaction

被引:22
|
作者
Wang, Qian [1 ]
Wang, Lei [2 ]
Wang, Hui [1 ]
Li, Zengxi [1 ]
Wu, Hui [2 ]
Li, Guangming [2 ]
Zhang, Xiangping [2 ]
Zhang, Suojiang [2 ]
机构
[1] Chinese Acad Sci, Grad Univ, Coll Chem & Chem Engn, Beijing 10049, Peoples R China
[2] Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China
来源
基金
国家高技术研究发展计划(863计划);
关键词
molecular sieve; SAPO-34; solid acid catalysts; methanol-to-olefin reaction; MTO process; TEA; template concentration; crystallization time; CRYSTALLIZATION; CONVERSION; SILICOALUMINOPHOSPHATE; DIETHYLAMINE; FRAMEWORK; ZEOLITES; TEMPLATE; CRYSTALS; SYSTEM;
D O I
10.1002/apj.453
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
The methanol-to-olefin (MTO) process is important because it offers an alternative to the conventional oil route for the conversion of natural gas or coal to light olefins. The most promising catalysts for the MTO reaction are solid acids with a zeolite structure, where reactants and products such as ethylene and propylene may freely diffuse through active catalysts, but products with larger kinetic diameters are trapped within the cages. In this work, SAPO-34 molecular sieves were synthesized by hydrothermal crystallization, using triethylamine (TEA) as the template. These samples were characterized by X-ray diffraction, scanning electron microscopy, thermo-gravimetric analysis-differential scanning calorimetry, energy dispersive spectroscopy, Fourier transform-infrared (FT-IR) and N(2) adsorption-desorption. The effects of template concentration and crystallization time on the physicochemical properties and catalytic performance were investigated. The crystallinity and morphology of SAPO-34 were influenced by the concentration of the template. Pure SAPO-34 was obtained when the TEA/Al(2)O(3) molar ratio was higher than 2.0. With increased crystallization time, the Si content in SAPO-34 crystals increased, which influenced the surface acidity. FT-IR spectra indicated that all samples were dominated by Lewis acid sites and the sample crystallized for 11 h exhibited the lowest number of Lewis acid sites. The catalytic performance of SAPO-34 was tested with the MTO reaction. High selectivity to olefins (C(2)H(4) + C(3)H(6)) was obtained over the catalyst synthesized with a TEA/Al(2)O(3) ratio of 3.0 and crystallization time of 11 h. At the reaction temperature of 450 degrees C, the methanol conversion approached 100% and the yield of C(2)-C(4) olefins was more than 80%. Hence, SAPO-34 molecular sieves were shown to be excellent catalysts for the MTO reaction. (C) 2010 Curtin University of Technology and John Wiley & Sons, Ltd.
引用
收藏
页码:596 / 605
页数:10
相关论文
共 50 条
  • [31] Synthesis and Applications of SAPO-34 Molecular Sieves
    Yu, Wenhe
    Wu, Xiaowen
    Cheng, Bohao
    Tao, Tianyi
    Min, Xin
    Mi, Ruiyu
    Huang, Zhaohui
    Fang, Minghao
    Liu, Yangai
    CHEMISTRY-A EUROPEAN JOURNAL, 2022, 28 (11)
  • [32] Synthesis and Characterization of ZnAPO-34 and SAPO-34: Effect of Zn on the Acidity and Catalytic Activity in the MTO Reaction
    Ruiz, Misael Garcia
    Aguilar Pliego, Julia
    Marquez Alvarez, Carlos
    Grande Casas, Marisol
    Sastre de Andres, Enrique
    JOURNAL OF THE MEXICAN CHEMICAL SOCIETY, 2021, 65 (01) : 61 - 73
  • [33] Busting the efficiency of SAPO-34 catalysts for the methanol-to-olefin conversion by post-synthesis methods
    Guoju Yang
    Ji Han
    Yujun Huang
    Xiaoxin Chen
    Valentin Valtchev
    Chinese Journal of Chemical Engineering, 2020, 28 (08) : 2022 - 2027
  • [34] Busting the efficiency of SAPO-34 catalysts for the methanol-to-olefin conversion by post-synthesis methods
    Yang, Guoju
    Han, Ji
    Huang, Yujun
    Chen, Xiaoxin
    Valtchev, Valentin
    CHINESE JOURNAL OF CHEMICAL ENGINEERING, 2020, 28 (08) : 2022 - 2027
  • [35] A green approach to improve the yield of SAPO-34 crystal as well as its methanol-to-olefin performance
    Duan, Ying
    Dai, Haowen
    Wang, Long-Sheng
    Zhang, Meng
    Wu, Li-Ming
    Ouyang, Gangfeng
    JOURNAL OF SOLID STATE CHEMISTRY, 2022, 309
  • [36] A Green and Cost-Effective Synthesis of Hierarchical SAPO-34 through Dry Gel Conversion and Its Performance in a Methanol-to-Olefin Reaction
    Li, Zhi-Hong
    Li, Xiao-Feng
    Di, Chun-Yu
    Dou, Tao
    Chen, Sheng-Li
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2021, 60 (43) : 15380 - 15390
  • [37] Nanosize-Enhanced Lifetime of SAPO-34 Catalysts in Methanol-to-Olefin Reactions
    Yang, Guoju
    Wei, Yingxu
    Xu, Shutao
    Chen, Jingrun
    Li, Jinzhe
    Li, Zhongmin
    Yu, Jihong
    Xu, Ruren
    JOURNAL OF PHYSICAL CHEMISTRY C, 2013, 117 (16): : 8214 - 8222
  • [38] Cobalt-isomorphous substituted SAPO-34 via milling and recrystallization for enhanced catalytic lifetime toward methanol-to-olefin reaction
    Lee, Su-Un
    Lee, You-Jin
    Kim, Jeong-Rang
    Jeong, Kwang-Eun
    Jeong, Soon-Yong
    JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY, 2019, 79 : 443 - 451
  • [39] The recyclable synthesis of hierarchical zeolite SAPO-34 with excellent MTO catalytic performance
    Xi, Dongyang
    Sun, Qiming
    Chen, Xiaoxin
    Wang, Ning
    Yu, Jihong
    CHEMICAL COMMUNICATIONS, 2015, 51 (60) : 11987 - 11989
  • [40] Dual Templating Fabrication of Hollow SAPO-34 Molecular Sieves for Enhanced MTO Catalytic Activity and Selectivity
    Yang, Hong
    Miao, Ping
    Sun, Qi
    Zhang, Yi
    Tian, Dayong
    CRYSTAL RESEARCH AND TECHNOLOGY, 2019, 54 (02)