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Title: Fischer-Tropsch Synthesis: Influence of CO Conversion on Selectivities H2/CO Usage Ratios and Catalyst Stability for a 0.27 percent Ru 25 percent Co/Al2O3 using a Slurry Phase Reactor

Abstract

The effect of CO conversion on hydrocarbon selectivities (i.e., CH{sub 4}, C{sub 5+}, olefin and paraffin), H{sub 2}/CO usage ratios, CO{sub 2} selectivity, and catalyst stability over a wide range of CO conversion (12-94%) on 0.27%Ru-25%Co/Al{sub 2}O{sub 3} catalyst was studied under the conditions of 220 C, 1.5 MPa, H{sub 2}/CO feed ratio of 2.1 and gas space velocities of 0.3-15 NL/g-cat/h in a 1-L continuously stirred tank reactor (CSTR). Catalyst samples were withdrawn from the CSTR at different CO conversion levels, and Co phases (Co, CoO) in the slurry samples were characterized by XANES, and in the case of the fresh catalysts, EXAFS as well. Ru was responsible for increasing the extent of Co reduction, thus boosting the active site density. At 1%Ru loading, EXAFS indicates that coordination of Ru at the atomic level was virtually solely with Co. It was found that the selectivities to CH{sub 4}, C{sub 5+}, and CO{sub 2} on the Co catalyst are functions of CO conversion. At high CO conversions, i.e. above 80%, CH{sub 4} selectivity experienced a change in the trend, and began to increase, and CO{sub 2} selectivity experienced a rapid increase. H{sub 2}/CO usage ratio and olefin content were foundmore » to decrease with increasing CO conversion in the range of 12-94%. The observed results are consistent with water reoxidation of Co during FTS at high conversion. XANES spectroscopy of used catalyst samples displayed spectra consistent with the presence of more CoO at higher CO conversion levels.« less

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE SC OFFICE OF SCIENCE (SC)
OSTI Identifier:
1042149
Report Number(s):
BNL-97827-2012-JA
Journal ID: ISSN 1022-5528; TRN: US201212%%560
DOE Contract Number:  
DE-AC02-98CH10886
Resource Type:
Journal Article
Journal Name:
Topics in Catalysis
Additional Journal Information:
Journal Volume: 54; Journal Issue: 13-15; Journal ID: ISSN 1022-5528
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; ALKENES; CATALYSTS; FISCHER-TROPSCH SYNTHESIS; HYDROCARBONS; PARAFFIN; SPECTRA; SPECTROSCOPY; STABILITY; TANKS; WATER

Citation Formats

Ma, W, Jacobs, G, Ji, Y, Bhatelia, T, Bukur, D, Khalid, S, and Davis, B. Fischer-Tropsch Synthesis: Influence of CO Conversion on Selectivities H2/CO Usage Ratios and Catalyst Stability for a 0.27 percent Ru 25 percent Co/Al2O3 using a Slurry Phase Reactor. United States: N. p., 2011. Web. doi:10.1007/s11244-011-9699-5.
Ma, W, Jacobs, G, Ji, Y, Bhatelia, T, Bukur, D, Khalid, S, & Davis, B. Fischer-Tropsch Synthesis: Influence of CO Conversion on Selectivities H2/CO Usage Ratios and Catalyst Stability for a 0.27 percent Ru 25 percent Co/Al2O3 using a Slurry Phase Reactor. United States. https://doi.org/10.1007/s11244-011-9699-5
Ma, W, Jacobs, G, Ji, Y, Bhatelia, T, Bukur, D, Khalid, S, and Davis, B. Sat . "Fischer-Tropsch Synthesis: Influence of CO Conversion on Selectivities H2/CO Usage Ratios and Catalyst Stability for a 0.27 percent Ru 25 percent Co/Al2O3 using a Slurry Phase Reactor". United States. https://doi.org/10.1007/s11244-011-9699-5.
@article{osti_1042149,
title = {Fischer-Tropsch Synthesis: Influence of CO Conversion on Selectivities H2/CO Usage Ratios and Catalyst Stability for a 0.27 percent Ru 25 percent Co/Al2O3 using a Slurry Phase Reactor},
author = {Ma, W and Jacobs, G and Ji, Y and Bhatelia, T and Bukur, D and Khalid, S and Davis, B},
abstractNote = {The effect of CO conversion on hydrocarbon selectivities (i.e., CH{sub 4}, C{sub 5+}, olefin and paraffin), H{sub 2}/CO usage ratios, CO{sub 2} selectivity, and catalyst stability over a wide range of CO conversion (12-94%) on 0.27%Ru-25%Co/Al{sub 2}O{sub 3} catalyst was studied under the conditions of 220 C, 1.5 MPa, H{sub 2}/CO feed ratio of 2.1 and gas space velocities of 0.3-15 NL/g-cat/h in a 1-L continuously stirred tank reactor (CSTR). Catalyst samples were withdrawn from the CSTR at different CO conversion levels, and Co phases (Co, CoO) in the slurry samples were characterized by XANES, and in the case of the fresh catalysts, EXAFS as well. Ru was responsible for increasing the extent of Co reduction, thus boosting the active site density. At 1%Ru loading, EXAFS indicates that coordination of Ru at the atomic level was virtually solely with Co. It was found that the selectivities to CH{sub 4}, C{sub 5+}, and CO{sub 2} on the Co catalyst are functions of CO conversion. At high CO conversions, i.e. above 80%, CH{sub 4} selectivity experienced a change in the trend, and began to increase, and CO{sub 2} selectivity experienced a rapid increase. H{sub 2}/CO usage ratio and olefin content were found to decrease with increasing CO conversion in the range of 12-94%. The observed results are consistent with water reoxidation of Co during FTS at high conversion. XANES spectroscopy of used catalyst samples displayed spectra consistent with the presence of more CoO at higher CO conversion levels.},
doi = {10.1007/s11244-011-9699-5},
url = {https://www.osti.gov/biblio/1042149}, journal = {Topics in Catalysis},
issn = {1022-5528},
number = 13-15,
volume = 54,
place = {United States},
year = {2011},
month = {12}
}