Effect of graphitic carbon modification on the catalytic performance of Fe@SiO2-GC catalysts for forming lower olefins via Fischer-Tropsch synthesis

被引:26
作者
Ni, Zhijiang [1 ]
Qin, Hengfei [2 ]
Kang, Shifei [3 ]
Bai, Jirong [1 ]
Wang, Zhilei [1 ]
Li, Yaguang [3 ]
Zheng, Zheng [1 ]
Li, Xi [1 ]
机构
[1] Fudan Univ, Dept Environm Sci & Engn, Shanghai 200433, Peoples R China
[2] Jiangsu Univ Technol, Sch Chem & Environm Engn, Jiangsu Key Lab E Waste Recycling, Changzhou 213001, Peoples R China
[3] Univ Shanghai Sci & Technol, Sch Environm & Architecture, Shanghai 200093, Peoples R China
基金
中国国家自然科学基金;
关键词
Fe@SiO2-GC; Core-shell; Graphitic carbon; Reducibility; Fischer-Tropsch synthesis; SUPPORTED IRON CATALYSTS; SELECTIVITY CONTROL; ACTIVATED CARBON; LIGHT OLEFINS; SYNTHESIS GAS; SURFACE; SILICA; COBALT; NANOPARTICLES; HYDROCARBONS;
D O I
10.1016/j.jcis.2018.01.017
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Mesoporous silica-encapsulated iron materials contribute to the suppression of self-aggregation and thereby enhances the Fischer-Tropsch synthesis activity. However, constructing Fe-based supported catalysts with high activity and selectivity in the Fischer-Tropsch synthesis to lower olefins (FM) by a conventional mesoporous silica support has been proven challenging due to its low hydrothermal stability and low reducibility. Herein, we developed a core-shell Fe@SiO2-GC structure with an optimized interface of the catalyst by introducing graphitic carbon (GC) that weakened the Fe-SiO2 interaction. Transmission electron microscopy and nitrogen adsorption-desorption characterization proved GC-modified catalysts had well-defined core-shell structures. The Fe@SiO2-GC-2 containing the optimal GC content had the largest surface area and pore volume, and outperformed Fe2O3@SiO2 in terms of CO conversion (60.1%) and C-2-C-4 olefin selectivity (40.7%) within 100 h. The significant improvement of FM performance was attributed to the rigid porous framework of GC, which allowed free access of syngas and inhibited mesoporous channel collapse during FTO, so the catalytic activity and stability were improved by the synergism between higher Fe dispersion and reducibility. Moreover, the narrow well-defined mesoporous channel also exerted a modest spatial restriction effect, which inhibited the formation of long-chain hydrocarbon and tailored the product distribution toward lower distillate, thus improving the selectivity toward C-2-C-4. (C) 2018 Elsevier Inc. All rights reserved.
引用
收藏
页码:16 / 22
页数:7
相关论文
共 54 条
  • [11] Effect of precursor on the catalytic performance of supported iron catalysts for the Fischer-Tropsch synthesis of lower olefins
    Galvis, Hirsa M. Torres
    Koeken, Ard C. J.
    Bitter, Johannes H.
    Davidian, Thomas
    Ruitenbeek, Matthijs
    Dugulan, A. Iulian
    de Jong, Krijn P.
    [J]. CATALYSIS TODAY, 2013, 215 : 95 - 102
  • [12] Iron Particle Size Effects for Direct Production of Lower Olefins from Synthesis Gas
    Galvis, Hirsa M. Torres
    Bitter, Johannes H.
    Davidian, Thomas
    Ruitenbeek, Matthijs
    Dugulan, A. Iulian
    de Jong, Krijn P.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (39) : 16207 - 16215
  • [13] Supported Iron Nanoparticles as Catalysts for Sustainable Production of Lower Olefins
    Galvis, Hirsa M. Torres
    Bitter, Johannes H.
    Khare, Chaitanya B.
    Ruitenbeek, Matthijs
    Dugulan, A. Iulian
    de Jong, Krijn P.
    [J]. SCIENCE, 2012, 335 (6070) : 835 - 838
  • [14] Morphology and surface properties of fumed silicas
    Gun'ko, VM
    Mironyuk, IF
    Zarko, VI
    Voronin, EF
    Turov, VV
    Pakhlov, EM
    Goncharuk, EV
    Nychiporuk, YM
    Vlasova, NN
    Gorbik, PP
    Mishchuk, OA
    Mishchuk, OA
    Chuiko, AA
    Kulik, TV
    Palyanytsya, BB
    Pakhovchishin, SV
    Skubiszewska-Zieba, J
    Janusz, W
    Turov, AV
    Leboda, R
    [J]. JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2005, 289 (02) : 427 - 445
  • [15] Ordered mesoporous carbon nanochannel reactors for high-performance Fischer-Tropsch synthesis
    Ha, Kyoung-Su
    Kwak, Geunjae
    Jun, Ki-Won
    Hwang, Jongkook
    Lee, Jinwoo
    [J]. CHEMICAL COMMUNICATIONS, 2013, 49 (45) : 5141 - 5143
  • [16] Surface Modification of Colloidal Silica Nanoparticles: Controlling the size and Grafting Process
    He, Wentao
    Wu, Danhua
    Li, Juan
    Zhang, Kai
    Xiang, Yushu
    Long, Lijuan
    Qin, Shuhao
    Yu, Jie
    Zhang, Qin
    [J]. BULLETIN OF THE KOREAN CHEMICAL SOCIETY, 2013, 34 (09) : 2747 - 2752
  • [17] The Mechanism of Potassium Promoter: Enhancing the Stability of Active Surfaces
    Huo, Chun-Fang
    Wu, Bao-Shan
    Gao, Peng
    Yang, Yong
    Li, Yong-Wang
    Jiao, Haijun
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (32) : 7403 - 7406
  • [18] FISCHER-TROPSCH SYNTHESIS ON COBALT AND RUTHENIUM - METAL DISPERSION AND SUPPORT EFFECTS ON REACTION-RATE AND SELECTIVITY
    IGLESIA, E
    SOLED, SL
    FIATO, RA
    [J]. JOURNAL OF CATALYSIS, 1992, 137 (01) : 212 - 224
  • [19] SELECTIVITY CONTROL AND CATALYST DESIGN IN THE FISCHER-TROPSCH SYNTHESIS - SITES, PELLETS, AND REACTORS
    IGLESIA, E
    REYES, SC
    MADON, RJ
    SOLED, SL
    [J]. ADVANCES IN CATALYSIS, VOL 39, 1993, 39 : 221 - 302
  • [20] Cyclopentadienyl surface as a support for zirconium polyethylene catalysts
    Iiskola, EI
    Timonen, S
    Pakkanen, TT
    Harkki, O
    Lehmus, P
    Seppala, JV
    [J]. MACROMOLECULES, 1997, 30 (10) : 2853 - 2859