Bifunctional Catalysts for One-Step Conversion of Syngas into Aromatics with Excellent Selectivity and Stability

被引:481
作者
Cheng, Kang [1 ]
Zhou, Wei [1 ]
Kang, Jincan [1 ]
He, Shun [1 ]
Shi, Shulin [1 ]
Zhang, Qinghong [1 ]
Pan, Yang [2 ]
Wen, Wu [2 ]
Wang, Ye [1 ]
机构
[1] Xiamen Univ, Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Lab Green Chem Product Alcohols Ethers, State Key Lab Phys Chem Solid Surfaces,Coll Chem, Xiamen 361005, Peoples R China
[2] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China
来源
CHEM | 2017年 / 3卷 / 02期
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
FISCHER-TROPSCH SYNTHESIS; SYNTHESIS GAS; METHANOL SYNTHESIS; LOWER OLEFINS; PROPANE AROMATIZATION; PRODUCT SELECTIVITY; ZIRCONIUM DIOXIDE; CO2; CONVERSION; ACTIVE-SITES; LIQUID FUELS;
D O I
10.1016/j.chempr.2017.05.007
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Syngas (CO/H-2) is a key platform for chemical utilization of non-petroleum carbon resources. Among syngas transformation routes, the direct synthesis of aromatics, which are among the most important bulk chemicals, is less successful because of the limited selectivity and poor catalyst stability. We report a successful design of bifunctional catalysts composed of Zn-doped ZrO2 nanoparticles dispersed on zeolite H-ZSM-5 for one-step conversion of syngas to aromatics with high selectivity and stability. Aromatics with 80% selectivity at CO conversion of 20% were achieved, and there was no catalyst deactivation in 1,000 hr. Methanol and dimethyl ether were formed as major intermediates on Zn-doped ZrO2, which were subsequently converted into aromatics on H-ZSM-5 via olefins. We discovered a self-promotion mechanism of CO in the selective formation of aromatics. As well as being a reactant, CO facilitates the removal of hydrogen species formed on H-ZSM-5 in the dehydrogenative aromatization of olefins.
引用
收藏
页码:334 / 347
页数:14
相关论文
共 70 条
  • [1] HYDROGEN ON ZINC-OXIDE - THEORY OF ITS HETEROLYTIC ADSORPTION
    ANDERSON, AB
    NICHOLS, JA
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1986, 108 (16) : 4742 - 4746
  • [2] A core/shell catalyst produces a spatially confined effect and shape selectivity in a consecutive reaction
    Bao, Jun
    He, Jingjiang
    Zhang, Yi
    Yoneyama, Yoshiharu
    Tsubaki, Noritatsu
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (02) : 353 - 356
  • [3] INTERMEDIATE SPECIES ON ZIRCONIA SUPPORTED METHANOL AEROGEL CATALYSTS .1. STATE OF THE CATALYST SURFACE BEFORE AND AFTER THE ADSORPTION OF HYDROGEN
    BIANCHI, D
    GASS, JL
    KHALFALLAH, M
    TEICHNER, SJ
    [J]. APPLIED CATALYSIS A-GENERAL, 1993, 101 (02) : 297 - 315
  • [4] Reaction pathways and rate-determining steps in reactions of alkanes on H-ZSM5 and Zn/H-ZSM5 catalysts
    Biscardi, JA
    Iglesia, E
    [J]. JOURNAL OF CATALYSIS, 1999, 182 (01) : 117 - 128
  • [5] The effect of a higher operating temperature on the Fischer-Tropsch/HZSM-5 bifunctional process
    Botes, FG
    [J]. APPLIED CATALYSIS A-GENERAL, 2005, 284 (1-2) : 21 - 29
  • [6] Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries
    Centi, Gabriele
    Quadrelli, Elsje Alessandra
    Perathoner, Siglinda
    [J]. ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (06) : 1711 - 1731
  • [7] Chang, 1978, U.S. Patent, Patent No. [4,096,163A, 4096163]
  • [8] Direct and Highly Selective Conversion of Synthesis Gas into Lower Olefins: Design of a Bifunctional Catalyst Combining Methanol Synthesis and Carbon-Carbon Coupling
    Cheng, Kang
    Gu, Bang
    Liu, Xiaoliang
    Kang, Jincan
    Zhang, Qinghong
    Wang, Ye
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (15) : 4725 - 4728
  • [9] Amphiphilic organosilane-directed synthesis of crystalline zeolite with tunable mesoporosity
    Choi, Minkee
    Cho, Hae Sung
    Srivastava, Rajendra
    Venkatesan, Chithravel
    Choi, Dae-Heung
    Ryoo, Ryong
    [J]. NATURE MATERIALS, 2006, 5 (09) : 718 - 723
  • [10] H-gallosilicate (MFI) propane aromatization catalyst: Influence of Si/Ga ratio on acidity, activity and deactivation due to coking
    Choudhary, VR
    Kinage, AK
    Sivadinarayana, C
    Devadas, P
    Sansare, SD
    Guisnet, M
    [J]. JOURNAL OF CATALYSIS, 1996, 158 (01) : 34 - 50