Temperature-dependent secondary conversion of primary products from methanol aromatization in a two-stage fluidized bed

被引:14
作者
Chen, Zhaohui [1 ]
Song, Wenlong [1 ]
Hou, Yilin [1 ]
Wang, Huiqiu [1 ]
Zhang, Chenxi [1 ]
Wang, Jian [1 ]
Yang, Yifeng [1 ]
Qian, Weizhong [1 ]
机构
[1] Tsinghua Univ, Dept Chem Engn, Beijing 100084, Peoples R China
关键词
Methanol to aromatics; Secondary conversion; Fluid Zn/ZSM-5 catalyst; Regional functionalization; Fluidized bed; HIGH-QUALITY TAR; CATALYTIC PERFORMANCE; HYDROGEN-TRANSFER; HYDROTHERMAL SYNTHESIS; FORMATION MECHANISM; AROMATICS; HYDROCARBONS; ZEOLITE; ZSM-5; H-ZSM-5;
D O I
10.1016/j.fuel.2020.117204
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Methanol to aromatics (MTA) following dual cycles concept unavoidably produced considerable amounts of olefinic intermediates and paraffinic by-products. Their formation and further conversion were vital to improving aromatics production. In this study, a two-stage fluid bed packed with fluid Zn/ZSM-5 catalyst in each stage was used to investigate the MTA reaction at 470 degrees C in the first stage and the secondary conversion of MTA primary products at temperatures from 270 degrees C to 550 degrees C in the second stage with time on stream. During the MTA reaction, the decrease of catalyst acidity was beneficial to controlling hydrogen transfer, thus blocking propane formation. During the secondary conversion of MTA products, at temperatures below 390 degrees C, the alkylation and hydrogen transfer reactions dominated and thus olefins were converted into more alkylbenzene as well as the undesired propane and butane. As the temperature increased from 430 degrees C to 550 degrees C, the aromatization of light hydrocarbon and the dealkylation of alkylbenzene were facilitated, producing more benzene and toluene but increasing methane and ethane yields. Meanwhile, the dehydrogenation and cracking of propane and butane were favored by high temperature and strong acidity so that the yields of ethene and propene increased. It was clarified that the characteristics of secondary conversion of MTA products varied and depended on reaction temperature and catalyst acidity. Based on these findings, the concept of regional functionalization of fluidized bed reactor was proposed for intensification of MTA process based on the reconfiguration of the temperature and acidity of catalyst stream during the fluidized bed reaction-regeneration cycle.
引用
收藏
页数:9
相关论文
共 42 条
  • [1] Theoretical study of the methylbenzene side-chain hydrocarbon pool mechanism in methanol to olefin catalysis
    Arstad, B
    Nicholas, JB
    Haw, JF
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (09) : 2991 - 3001
  • [2] Highly selective conversion of methanol to propylene: design of an MFI zeolite with selective blockage of (010) surfaces
    Cai, Dali
    Wang, Ning
    Chen, Xiao
    Ma, Yunhai
    Hou, Yilin
    Li, Xinghua
    Zhang, Chenxi
    Chen, Zhaohui
    Song, Wenlong
    Arslan, Muhammad Tahir
    Li, Yiru
    Wang, Yao
    Qian, Weizhong
    Wei, Fei
    [J]. NANOSCALE, 2019, 11 (17) : 8096 - 8101
  • [3] A multi-stage fluidized bed strategy for the enhanced conversion of methanol into aromatics
    Chen, Zhaohui
    Hou, Yilin
    Yang, Yifeng
    Cai, Dali
    Song, Wenlong
    Wang, Ning
    Qian, Weizhong
    [J]. CHEMICAL ENGINEERING SCIENCE, 2019, 204 : 1 - 8
  • [4] High-yield production of aromatics from methanol using a temperature-shifting multi-stage fluidized bed reactor technology
    Chen, Zhaohui
    Hou, Yilin
    Song, Wenlong
    Cai, Dali
    Yang, Yifeng
    Cui, Yu
    Qian, Weizhong
    [J]. CHEMICAL ENGINEERING JOURNAL, 2019, 371 : 639 - 646
  • [5] Coupling coal pyrolysis with char gasification in a multi-stage fluidized bed to co-produce high-quality tar and syngas
    Chen, Zhaohui
    Li, Yunjia
    Lai, Dengguo
    Geng, Sulong
    Zhou, Qi
    Gao, Shiqiu
    Xu, Guangwen
    [J]. APPLIED ENERGY, 2018, 215 : 348 - 355
  • [6] Simultaneous production of CH4-rich syngas and high-quality tar from lignite by the coupling of noncatalytic/catalytic pyrolysis and gasification in a pressurized integrated fluidized bed
    Chen, Zhaohui
    Gao, Shiqiu
    Xu, Guangwen
    [J]. APPLIED ENERGY, 2017, 208 : 1527 - 1537
  • [7] Chowdhury A. D., 2018, ANGEW CHEM, V130, P8227, DOI [10.1002/ange.201803279, DOI 10.1002/ANGE.201803279]
  • [8] Modified zeolite ZSM-5 for the methanol to aromatics reaction
    Conte, Marco
    Lopez-Sanchez, Jose A.
    He, Qian
    Morgan, David J.
    Ryabenkova, Yulia
    Bartley, Jonathan K.
    Carley, Albert F.
    Taylor, Stuart H.
    Kiely, Christopher J.
    Khalid, Karim
    Hutchings, Graham J.
    [J]. CATALYSIS SCIENCE & TECHNOLOGY, 2012, 2 (01) : 105 - 112
  • [9] Developing NHC-Iridium Catalysts for the Highly Efficient Enantioselective Intramolecular Hydroamination Reaction
    Gao, Pengchao
    Sipos, Gellert
    Foster, Daven
    Dorta, Reto
    [J]. ACS CATALYSIS, 2017, 7 (09): : 6060 - 6064
  • [10] Mechanism of the Catalytic Conversion of Methanol to Hydrocarbons
    Ilias, Samia
    Bhan, Aditya
    [J]. ACS CATALYSIS, 2013, 3 (01): : 18 - 31