期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 12, 期 19, 页码 5814-5828出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy00988a
关键词
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资金
- Next Generation Carbon Upcycling Project through the National Research Foundation (NRF) - Ministry of Science and ICT, Republic of Korea [NRF-2017M1A2A2043110]
- C1 Gas Refinery Program through the National Research Foundation of Korea (NRF) - Ministry of Science, ICT & Future Planning [NRF-2017M3D3A1A01037001]
- KRICT Project of the Korea Research Institute of Chemical Technology [SI2212-10]
We demonstrated two design methods for improving the olefin selectivity in Fischer-Tropsch synthesis reactions using Fe catalysts supported on SiO2. Fe/SiO2 catalysts synthesized through classical impregnation and Fe-SiO2 catalysts synthesized through impregnation followed by calcination were obtained. The Fe-SiO2 catalysts showed higher selectivity for C2-C4 olefins compared to Fe/SiO2 catalysts, even with a high Fe loading. The interactions between Fe-SiO2 catalysts and SiO2 were identified to be moderate in strength.
We demonstrated two design methods for obtaining Fe catalysts to improve the olefin selectivity in Fischer-Tropsch synthesis (FTS) reactions through the use of a SiO2 support. Fe/SiO2 catalysts, synthesized through classical impregnation, and Fe-SiO2 catalysts, synthesized through impregnation followed by calcination at 1700 degrees C, with Fe loadings of 1, 5, and 10 wt% were obtained. The Fe-SiO2 catalysts achieved C2-C4 olefins in C2-C4 hydrocarbons, O/(O + P), of 62.5-73.0%, whereas the O/(O + P) of the Fe/SiO2 catalysts decreased significantly with high Fe loadings. Using various characterization techniques, the main carbide species was identified to be Fe5C2, and based on the crystal size and composition of the Fe species, it was concluded that the interactions of Fe-SiO2 catalysts with SiO2 are of moderate strength. The iron time yield of C2-C4 olefins (FTYC2-C4 olefins) as a function of the Fe5C2 composition was higher for the Fe-SiO2 catalysts than for the Fe/SiO2 catalysts with corresponding Fe loadings; the highest value obtained for 1 wt% Fe-SiO2 was a factor of 3.5 higher than that of 1 wt% Fe/SiO2. The reaction results showed that the C2-C4 olefins can be selectively produced using the Fe-SiO2 catalyst even with a high Fe content. A density functional theory (DFT) study was performed to investigate the effect of SiO2 promotion on Fe carbides, and it was concluded that SiO2 promotion resulted in high selectivity for olefins, CH4, and CO2. To suppress CH4 or CO2 formation and boost CO conversion, Na-added catalysts with various Na ratios were tested, and successfully reduced CH4 selectivity and enhanced CO conversion.
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