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Co-precipitated Fe-Zr catalysts for the Fischer-Tropsch synthesis of lower olefins (C2O ∼ C4O): Synergistic effects of Fe and Zr
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DOI：10.1016/j.jcat.2019.08.037.png)
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Abstract
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Synthesis of lower olefins using syngas (H-2/CO) in a fixed-bed reactor under 1.0 MPa, WHSV = 3 NLH2/CO center dot g(Fe)(-1) center dot h(-1) (WHSV = 3 NLH2/CO center dot g(Fe)(-1) center dot h(-1) for Zr-p), H-2/CO = 2 was investigated over a series of Fe-based catalysts with Zr as the promoter. The catalysts were prepared by co-precipitation (Fe and Zr) and K was impregnated into the precipitate. The prepared catalysts with different Zr/Fe mol ratio (Zr-0, Zr-0.2, Zr-1, Zr-2 and Zr-p) were characterized by N-2 adsorption/desorption, X-ray diffraction (XRD), Raman spectroscopy (Raman), temperature-programmed reduction (TPR) and X-ray photoelectron spectroscopy (XPS). Synergistic effects of Fe and Zr on the nanostructure, textural, surface property and catalytic performance were analyzed. Characterization of the catalyst showed that the introduction of ZrO2 is in favor of the formation of mesopores due to the inhibition between Fe and Zr on each other's crystal growth, increasing alpha-Fe2O3 dispersion and the proportion of surface reduction to bulk reduction, which makes the catalysts easily be reduced by H-2 and CO. However, the interaction between Fe and Zr significantly suppresses the formation of theta-Fe3C and carbon deposition of catalysts. The optimal Fe/Zr mole ratio of Zr-X catalysts is found to be 1/1 due to the synergistic effect of Fe and Zr, the improved distribution of alpha-Fe2O3 and the abundant defects on alpha-Fe2O3 in the catalyst. In the case of Zr-1, the CO conversion and the selectivity toward lower olefins reached 82.1% and 34.6% at 270 degrees C. Adequate Zr, acting as a block of chain growth and weakening the adsorption of light olefins on active sites, is essential to improve the light olefins selectivity. (C) 2019 Elsevier Inc. All rights reserved.
Keywords:
Fe-Zr catalysts
Synergistic effect
Fischer-Tropsch to Olefins
Zr/Fe molar ratio
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