Inverse kinetic isotope effects and deuterium enrichment as a function of carbon number during formation of C–C bonds in cobalt catalyzed Fischer–Tropsch synthesis

Shi, Bingbing; Jin, Chunfen

doi:10.1016/j.apcata.2010.11.039

Cited by 30 publications

(21 citation statements)

References 31 publications

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“…It has been reported that during Co catalyzed FT reactions the CO conversion is always higher when H 2 was replaced by D 2 under the same reaction conditions, indicating that there is an inverse isotope effect [15]. This effect was also reported for Ru and Fe catalyzed FT reactions [19][20][21][22].…”

Section: Inverse Isotope Effect During Iron Catalyzed Ft Reactionmentioning

confidence: 60%

“…This mechanism has been used to explain the inverse isotope effect, the deuterium enrichment in hydrocarbons, and the formation of 1-alkenes, alkanes [15,16] and branched hydrocarbons [8]. In this study, we provide evidence to show that the formation of 2-alkenes is through a different pathway from 1-alkenes based on results of H 2 /D 2 switching experiments of FT reactions over iron catalysts.…”

Section: Introductionmentioning

confidence: 85%

“…The Fischer-Tropsch synthesis procedure is the same as described previously [15]. In a typical run, 1.5 g of iron catalyst (Fe:Si:K = 100:4.6:1.4) is used.…”

Section: Methodsmentioning

confidence: 99%

“…This procedure was usually repeated two times under one set of reaction conditions. Liquid samples were analyzed by GC and the identities of products were confirmed by GC/MS [15,18].…”

Section: Methodsmentioning

confidence: 99%

“…Based on isotope tracer results, we proposed a modified alkylidene mechanism for the FT reaction over cobalt catalysts [15,16]. This mechanism can also be used to explain the isotope tracer results of FT reactions over iron catalysts.…”

Section: Inverse Isotope Effect During Iron Catalyzed Ft Reactionmentioning

confidence: 98%

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Formation of 2-alkenes as secondary products during Fischer–Tropsch synthesis

Shi

Liao

Naumovitz

2015

Applied Catalysis A: General

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Section: Inverse Isotope Effect During Iron Catalyzed Ft Reactionmentioning

confidence: 60%

Section: Introductionmentioning

confidence: 85%

“…The Fischer-Tropsch synthesis procedure is the same as described previously [15]. In a typical run, 1.5 g of iron catalyst (Fe:Si:K = 100:4.6:1.4) is used.…”

Section: Methodsmentioning

confidence: 99%

“…This procedure was usually repeated two times under one set of reaction conditions. Liquid samples were analyzed by GC and the identities of products were confirmed by GC/MS [15,18].…”

Section: Methodsmentioning

confidence: 99%

Section: Inverse Isotope Effect During Iron Catalyzed Ft Reactionmentioning

confidence: 98%

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Formation of 2-alkenes as secondary products during Fischer–Tropsch synthesis

Shi

Liao

Naumovitz

2015

Applied Catalysis A: General

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Methane Steam Reforming over a Ni/NiAl₂O₄ Model Catalyst—Kinetics

2014

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The steam reforming reaction of methane to synthesis gas (CO and H2) was investigated in a very broad steam‐to‐carbon (S/C) ratio range (0.2–7.1) over a Ni/NiAl2O4 catalyst at 843, 858, and 873 K. The dataset includes 179 data points at each temperature giving a detailed insight in the gradual change of kinetic orders in both methane and steam with changing S/C ratios as well as with total reactant partial pressures at differential conversion levels. At low S/C ratios, steam dominates the kinetics with high kinetic orders (low for methane) and vice versa for methane at high S/C ratios. The extent of the water gas shift reaction was assessed by 13CO2 co‐feed experiments and thermodynamic modelling and found to be not in equilibrium. A change in the kinetic isotope effect (i.e., inverse and normal), as well as the apparent activation energy, was observed depending on the applied S/C ratios. The experimental data were satisfactorily described by a Langmuir–Hinshelwood expression.

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Fischer‐Tropsch synthesis: Effect of solvent on the H₂‐D₂ isotopic exchange rate over an activated cobalt catalyst

et al. 2016

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The effect of solvent on the hydrogen-deuterium isotopic homomolecular exchange over a traditional Fischer-Tropsch cobalt catalyst (25 % Co/Al 2 O 3 ) was investigated using a plug flow reactor at two different reaction temperatures (room temperature (26 8C) and -20 8C) and at atmospheric pressure. In this study, three different solvents were tested, including n-pentane, n-hexadecane, and C-30 oil. The consumption of H 2 and D 2 is the same, and the concentration of the HD produced is twice the consumption of H 2 or D 2 at dry (without solvent) conditions. At room temperature and at -20 8C, conditions without solvent exhibited 100 mol% exchange with the formation of H 2 :HD:D 2 having a 1:2:1 ratio. For n-pentane solvent, the exchange rates were $97 and $80 mol% at 26 and À20 8C, respectively. For the n-hexadecane and C 30 oil solvents, the initial exchange rate was $50 mol%, with the exchange rate decreasing over time. The lower exchange rate with the n-hexadecane and C 30 oil solvents, and also n-pentane at -20 8C, is likely due primarily to the limited mobility of reactant molecules in the liquid-filled pores of the catalyst. Blocking or covering of the pores of the catalyst depends on the molecular mass and density of the solvent. No isotopic partitioning preference was observed at two different temperatures and various solvents for the active cobalt catalyst.

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Inverse kinetic isotope effects and deuterium enrichment as a function of carbon number during formation of C–C bonds in cobalt catalyzed Fischer–Tropsch synthesis

Cited by 30 publications

References 31 publications

Formation of 2-alkenes as secondary products during Fischer–Tropsch synthesis

Formation of 2-alkenes as secondary products during Fischer–Tropsch synthesis

Methane Steam Reforming over a Ni/NiAl₂O₄ Model Catalyst—Kinetics

Fischer‐Tropsch synthesis: Effect of solvent on the H₂‐D₂ isotopic exchange rate over an activated cobalt catalyst

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Inverse kinetic isotope effects and deuterium enrichment as a function of carbon number during formation of C–C bonds in cobalt catalyzed Fischer–Tropsch synthesis

Cited by 30 publications

References 31 publications

Formation of 2-alkenes as secondary products during Fischer–Tropsch synthesis

Formation of 2-alkenes as secondary products during Fischer–Tropsch synthesis

Methane Steam Reforming over a Ni/NiAl2O4 Model Catalyst—Kinetics

Fischer‐Tropsch synthesis: Effect of solvent on the H2‐D2 isotopic exchange rate over an activated cobalt catalyst

Contact Info

Product

Resources

About

Methane Steam Reforming over a Ni/NiAl₂O₄ Model Catalyst—Kinetics

Fischer‐Tropsch synthesis: Effect of solvent on the H₂‐D₂ isotopic exchange rate over an activated cobalt catalyst