Davis, Burtron H.

Link to this page

Authority KeyName Variants
fffb46c1-32d7-4d61-834c-dd253b8c8463
  • Davis, Burtron H. (2)
Projects

Author's Bibliography

Quantitative comparison of iron and cobalt based catalysts for the Fischer-Tropsch synthesis under clean and poisoning conditions

Ma, Wenping; Jacobs, Gary; Sparks, Dennis E.; Todić, Branislav; Bukur, Dragomir B.; Davis, Burtron H.

(Elsevier, Amsterdam, 2020)

TY  - JOUR
AU  - Ma, Wenping
AU  - Jacobs, Gary
AU  - Sparks, Dennis E.
AU  - Todić, Branislav
AU  - Bukur, Dragomir B.
AU  - Davis, Burtron H.
PY  - 2020
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/4484
AB  - Quantitative data comparing iron and cobalt based catalysts for the Fischer-Tropsch synthesis (FTS) are scarce due to the fact that these two kinds of catalysts typically utilize different process conditions. This paper focuses on studying the catalytic behavior of two highly active iron and cobalt based research catalysts at clean conditions and during poisoning with common syngas contaminants. The catalyst activity and selectivity at identical conditions, the CO conversion effect, and the effect of poisons on iron and cobalt catalysts were systematically explored in a quantitative manner. At a set of identical FTS conditions, the cobalt catalyst was 2.5 times as active as the iron catalyst with higher CH4 and C-5+ selectivities but much less olefins and lower CO2 selectivity. Cobalt based catalysts are more susceptible to deactivation by oxidation at high CO conversions (e.g.  gt  80%) due to the high partial pressure of water (P-H2O) in the reactor, while the iron catalyst can be stabilized at a high conversion level. Under clean FTS conditions, the cobalt catalysts displayed a more pronounced CO conversion effect on stability and selectivity; on the other hand, a combination of effects (i.e. from CO conversion and the nature of the catalyst) were observed for the iron catalysts. The sensitivities of the Fe and Co catalysts to the typical contaminants (i.e., H2S and NH3) present in the syngas derived from coal, natural gas or biomass were compared. Iron and cobalt catalysts exhibited similar resistance to the H2S poison (i.e. threshold levels 25-50 ppb), but the iron catalyst was found to be much more resistant to ammonia than the cobalt catalyst (i.e., threshold levels of 80 ppm and 45 ppb, respectively). Co-feeding 150-200 ppm ammonia lowered CH4 selectivity and 2-olefin content (suppressing secondary reactions of 1-olefin) on both types of catalysts. In contrast, co-feeding up to 1 ppm H2S significantly increased CH4 formation only on cobalt catalysts but had a minor effect on CH4 selectivity with iron catalysts. It increased 2-olefin content (enhanced secondary reactions of 1-olefin) regardless of catalyst type. H2S and NH3 have different impacts on H-2, CO adsorption, and the formation of sulfur and nitride compounds have been proposed to explain these dissimilar effects.
PB  - Elsevier, Amsterdam
T2  - Catalysis Today
T1  - Quantitative comparison of iron and cobalt based catalysts for the Fischer-Tropsch synthesis under clean and poisoning conditions
EP  - 136
SP  - 125
VL  - 343
DO  - 10.1016/j.cattod.2019.04.011
ER  - 
@article{
author = "Ma, Wenping and Jacobs, Gary and Sparks, Dennis E. and Todić, Branislav and Bukur, Dragomir B. and Davis, Burtron H.",
year = "2020",
abstract = "Quantitative data comparing iron and cobalt based catalysts for the Fischer-Tropsch synthesis (FTS) are scarce due to the fact that these two kinds of catalysts typically utilize different process conditions. This paper focuses on studying the catalytic behavior of two highly active iron and cobalt based research catalysts at clean conditions and during poisoning with common syngas contaminants. The catalyst activity and selectivity at identical conditions, the CO conversion effect, and the effect of poisons on iron and cobalt catalysts were systematically explored in a quantitative manner. At a set of identical FTS conditions, the cobalt catalyst was 2.5 times as active as the iron catalyst with higher CH4 and C-5+ selectivities but much less olefins and lower CO2 selectivity. Cobalt based catalysts are more susceptible to deactivation by oxidation at high CO conversions (e.g.  gt  80%) due to the high partial pressure of water (P-H2O) in the reactor, while the iron catalyst can be stabilized at a high conversion level. Under clean FTS conditions, the cobalt catalysts displayed a more pronounced CO conversion effect on stability and selectivity; on the other hand, a combination of effects (i.e. from CO conversion and the nature of the catalyst) were observed for the iron catalysts. The sensitivities of the Fe and Co catalysts to the typical contaminants (i.e., H2S and NH3) present in the syngas derived from coal, natural gas or biomass were compared. Iron and cobalt catalysts exhibited similar resistance to the H2S poison (i.e. threshold levels 25-50 ppb), but the iron catalyst was found to be much more resistant to ammonia than the cobalt catalyst (i.e., threshold levels of 80 ppm and 45 ppb, respectively). Co-feeding 150-200 ppm ammonia lowered CH4 selectivity and 2-olefin content (suppressing secondary reactions of 1-olefin) on both types of catalysts. In contrast, co-feeding up to 1 ppm H2S significantly increased CH4 formation only on cobalt catalysts but had a minor effect on CH4 selectivity with iron catalysts. It increased 2-olefin content (enhanced secondary reactions of 1-olefin) regardless of catalyst type. H2S and NH3 have different impacts on H-2, CO adsorption, and the formation of sulfur and nitride compounds have been proposed to explain these dissimilar effects.",
publisher = "Elsevier, Amsterdam",
journal = "Catalysis Today",
title = "Quantitative comparison of iron and cobalt based catalysts for the Fischer-Tropsch synthesis under clean and poisoning conditions",
pages = "136-125",
volume = "343",
doi = "10.1016/j.cattod.2019.04.011"
}
Ma, W., Jacobs, G., Sparks, D. E., Todić, B., Bukur, D. B.,& Davis, B. H.. (2020). Quantitative comparison of iron and cobalt based catalysts for the Fischer-Tropsch synthesis under clean and poisoning conditions. in Catalysis Today
Elsevier, Amsterdam., 343, 125-136.
https://doi.org/10.1016/j.cattod.2019.04.011
Ma W, Jacobs G, Sparks DE, Todić B, Bukur DB, Davis BH. Quantitative comparison of iron and cobalt based catalysts for the Fischer-Tropsch synthesis under clean and poisoning conditions. in Catalysis Today. 2020;343:125-136.
doi:10.1016/j.cattod.2019.04.011 .
Ma, Wenping, Jacobs, Gary, Sparks, Dennis E., Todić, Branislav, Bukur, Dragomir B., Davis, Burtron H., "Quantitative comparison of iron and cobalt based catalysts for the Fischer-Tropsch synthesis under clean and poisoning conditions" in Catalysis Today, 343 (2020):125-136,
https://doi.org/10.1016/j.cattod.2019.04.011 . .
1
37
6
36

Kinetic Modeling of Secondary Methane Formation and 1-Olefin Hydrogenation in Fischer-Tropsch Synthesis over a Cobalt Catalyst

Todić, Branislav; Ma, Wenping; Jacobs, Gary; Nikačević, Nikola; Davis, Burtron H.; Bukur, Dragomir B.

(Wiley, Hoboken, 2017)

TY  - JOUR
AU  - Todić, Branislav
AU  - Ma, Wenping
AU  - Jacobs, Gary
AU  - Nikačević, Nikola
AU  - Davis, Burtron H.
AU  - Bukur, Dragomir B.
PY  - 2017
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/3678
AB  - A detailed kinetic model of Fischer-Tropsch synthesis (FTS) product formation, including secondary methane formation and 1-olefin hydrogenation, has been developed. Methane formation in FTS over the cobalt-based catalyst is well known to be higher-than-expected compared to other n-paraffin products under typical reaction conditions. A novel model proposes secondary methane formation on a different type of active site, which is not active in forming C2+ products, to explain this anomalous methane behavior. In addition, a model of secondary 1-olefin hydrogenation has also been developed. Secondary 1-olefin hydrogenation is related to secondary methane formation with both reactions happening on the same type of active sites. The model parameters were estimated from experimental data obtained with Co/Re/-Al2O3 catalyst in a slurry-phase stirred tank reactor over a range of conditions (T = 478, 493, and 503 K, P = 1.5 and 2.5 MPa, H-2/CO feed ratio = 1.4 and 2.1, and X-CO = 16-62%). The proposed model including secondary methane formation and 1-olefin hydrogenation is shown to provide an improved quantitative and qualitative prediction of experimentally observed behavior compared to the detailed model with only primary reactions.
PB  - Wiley, Hoboken
T2  - International Journal of Chemical Kinetics
T1  - Kinetic Modeling of Secondary Methane Formation and 1-Olefin Hydrogenation in Fischer-Tropsch Synthesis over a Cobalt Catalyst
EP  - 874
IS  - 12
SP  - 859
VL  - 49
DO  - 10.1002/kin.21133
ER  - 
@article{
author = "Todić, Branislav and Ma, Wenping and Jacobs, Gary and Nikačević, Nikola and Davis, Burtron H. and Bukur, Dragomir B.",
year = "2017",
abstract = "A detailed kinetic model of Fischer-Tropsch synthesis (FTS) product formation, including secondary methane formation and 1-olefin hydrogenation, has been developed. Methane formation in FTS over the cobalt-based catalyst is well known to be higher-than-expected compared to other n-paraffin products under typical reaction conditions. A novel model proposes secondary methane formation on a different type of active site, which is not active in forming C2+ products, to explain this anomalous methane behavior. In addition, a model of secondary 1-olefin hydrogenation has also been developed. Secondary 1-olefin hydrogenation is related to secondary methane formation with both reactions happening on the same type of active sites. The model parameters were estimated from experimental data obtained with Co/Re/-Al2O3 catalyst in a slurry-phase stirred tank reactor over a range of conditions (T = 478, 493, and 503 K, P = 1.5 and 2.5 MPa, H-2/CO feed ratio = 1.4 and 2.1, and X-CO = 16-62%). The proposed model including secondary methane formation and 1-olefin hydrogenation is shown to provide an improved quantitative and qualitative prediction of experimentally observed behavior compared to the detailed model with only primary reactions.",
publisher = "Wiley, Hoboken",
journal = "International Journal of Chemical Kinetics",
title = "Kinetic Modeling of Secondary Methane Formation and 1-Olefin Hydrogenation in Fischer-Tropsch Synthesis over a Cobalt Catalyst",
pages = "874-859",
number = "12",
volume = "49",
doi = "10.1002/kin.21133"
}
Todić, B., Ma, W., Jacobs, G., Nikačević, N., Davis, B. H.,& Bukur, D. B.. (2017). Kinetic Modeling of Secondary Methane Formation and 1-Olefin Hydrogenation in Fischer-Tropsch Synthesis over a Cobalt Catalyst. in International Journal of Chemical Kinetics
Wiley, Hoboken., 49(12), 859-874.
https://doi.org/10.1002/kin.21133
Todić B, Ma W, Jacobs G, Nikačević N, Davis BH, Bukur DB. Kinetic Modeling of Secondary Methane Formation and 1-Olefin Hydrogenation in Fischer-Tropsch Synthesis over a Cobalt Catalyst. in International Journal of Chemical Kinetics. 2017;49(12):859-874.
doi:10.1002/kin.21133 .
Todić, Branislav, Ma, Wenping, Jacobs, Gary, Nikačević, Nikola, Davis, Burtron H., Bukur, Dragomir B., "Kinetic Modeling of Secondary Methane Formation and 1-Olefin Hydrogenation in Fischer-Tropsch Synthesis over a Cobalt Catalyst" in International Journal of Chemical Kinetics, 49, no. 12 (2017):859-874,
https://doi.org/10.1002/kin.21133 . .
1
11
8
11