Fe-containing carbon obtained from ferrocene: Influence of the preparation procedure on the catalytic performance in FTS reaction

被引:12
作者
Cruz, Marcia G. A. [1 ,2 ]
de Oliveira, Ana Paula S. [2 ]
Fernandes, Fabiano A. N. [1 ]
de Sousa, Francisco F. [3 ,4 ]
Oliveira, Alcineia C. [2 ]
Filho, Josue M. [3 ]
Campos, Adriana F. [5 ]
Rodriguez-Castellon, Enrique [6 ]
机构
[1] Univ Fed Ceara, Dept Engn Quim, Campus Pici,Bloco 709, BR-60455760 Fortaleza, Ceara, Brazil
[2] Univ Fed Ceara, Dept Quim Analit & Fis Quim, Campus Pici,Bloco 940, BR-60455760 Fortaleza, Ceara, Brazil
[3] Univ Fed Ceara, Dept Fis, Campus Pici,Bloco 922, BR-60455760 Fortaleza, Ceara, Brazil
[4] Univ Fed Sul & Sudeste Para, Campus Univ Maraba, BR-68505080 Maraba, Para, Brazil
[5] Ctr Tecnol Estrateg Nordeste CETENE, Ave Prof Luiz Freire, BR-50740540 Recife, PE, Brazil
[6] Univ Malaga, Fac Ciencias, Dept Quim Inorgan, E-29071 Malaga, Spain
关键词
Ferrocene; Fe-doped nitrogen; Fischer Tropsch; Magnetite; Iron carbides; FISCHER-TROPSCH SYNTHESIS; POLYSTYRENE MESOPOROUS CARBON; NANO-CATALYST; NANOPARTICLES; COPRECIPITATION; ETHYLBENZENE; COMPOSITE; SUPPORT; RAMAN;
D O I
10.1016/j.cej.2017.02.047
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Four different preparation routes were applied to obtain Fe-containing carbon catalysts for Fischer Tropsch Synthesis (FTS) including copolymer assisted co-precipitation of iron precursor, chemical modification of ferrocene, sol-gel and wetness impregnation of iron on polymeric carbon. The effects of the FTS reaction temperature and pressure were also examined. Using ferrocene as a starting precursor and applying sol-gel method to prepare the solid, the syngas is readily converted to C-10(+) hydrocarbons with a conversion of up to 56% and a productivity of 34 mg (hyarocarboa).g(cat)(-1).h(-1) at 240 degrees C and 20 atm. Impregnation method gave a Fe/C based catalyst with the highest exposure of active sites, including surface Fe3+ and Fe2+ redox sites with great properties in FTS. Chemical modification of ferrocene route enables the formation of hematite and maghemite nanoparticles on carbon, which were in situ reduced to magnetite and iron carbides, being the latter mostly active for the water gas shift reaction. It is found that copolymer assisted co-precipitation of ferrocene facilitates the production of large crystals of magnetite, which suffered from sintering and coking exhibiting low performance in FTS. Among these methods, sol-gel based catalyst proved to have superior performance due to the good dispersion of Fe, stable magnetite and iron carbide and Fe-doped nitrogen carbon phases production. Based on spent catalysts characterizations, the synergetic effect between magnetite and the iron carbides phases in the sol-gel based catalyst plays an important role in heavy hydrocarbon formation. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:143 / 156
页数:14
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