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Mechanism of Cobalt-Catalyzed CO Hydrogenation: 2. Fischer-Tropsch Synthesis.

ABSTRACT: Fischer-Tropsch (FT) synthesis is one of the most complex catalyzed chemical reactions in which the chain-growth mechanism that leads to formation of long-chain hydrocarbons is not well understood yet. The present work provides deeper insight into the relation between the kinetics of the FT reaction on a silica-supported cobalt catalyst and the composition of the surface adsorbed layer. Cofeeding experiments of ¹²C₃H₆ with ¹³CO/H₂ evidence that CH _x surface intermediates are involved in chain growth and that chain growth is highly reversible. We present a model-based approach of steady-state isotopic transient kinetic analysis measurements at FT conditions involving hydrocarbon products containing up to five carbon atoms. Our data show that the rates of chain growth and chain decoupling are much higher than the rates of monomer formation and chain termination. An important corollary of the microkinetic model is that the fraction of free sites, which is mainly determined by CO pressure, has opposing effects on CO consumption rate and chain-growth probability. Lower CO pressure and more free sites leads to increased CO consumption rate but decreased chain-growth probability because of an increasing ratio of chain decoupling over chain growth. The preferred FT condition involves high CO pressure in which chain-growth probability is increased at the expense of the CO consumption rate.

SUBMITTER: Chen W

PROVIDER: S-EPMC5716444 | biostudies-literature | 2017 Dec

REPOSITORIES: biostudies-literature

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Mechanism of Cobalt-Catalyzed CO Hydrogenation: 2. Fischer-Tropsch Synthesis.

Chen Wei W Filot Ivo A W IAW Pestman Robert R Hensen Emiel J M EJM

ACS catalysis 20171016 12

Fischer-Tropsch (FT) synthesis is one of the most complex catalyzed chemical reactions in which the chain-growth mechanism that leads to formation of long-chain hydrocarbons is not well understood yet. The present work provides deeper insight into the relation between the kinetics of the FT reaction on a silica-supported cobalt catalyst and the composition of the surface adsorbed layer. Cofeeding experiments of 12C3H6 with 13CO/H2 evidence t ...[more]

PMID: 29226010

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Project description:Renewable liquid fuels production from landfill waste provides a promising alternative to conventional carbon-intensive waste management methods and has the potential to contribute to the transition toward low-carbon fuel pathways. In this work, we investigated the life cycle greenhouse gas (GHG) emissions of producing Fischer-Tropsch diesel from landfill gas (LFG) using the TriFTS catalytic conversion process and compared it to fossil-based petroleum diesel. A life cycle-based comparison was made between TriFTS diesel and other LFG waste management pathways, LFG-to-Electricity and LFG-to-Compressed renewable natural gas (RNG), on a per kilogram of feedstock basis as well as on a per MJ of energy basis, which also included the LFG-to-Direct Combustion pathway. The study considered flaring of LFG as the common underlying counterfactual scenario for all of the waste-to-energy product pathways. We estimated the life cycle GHG emissions for TriFTS diesel to be -36.4 carbon dioxide equivalent (grams CO2e)/MJ which is significantly lower than its fossil fuel counterpart which was estimated to be 90.5 g CO2e/MJ on a cradle-to-grave basis. The life cycle emission results from both perspectives (per kg feedstock and per MJ energy output) show that TriFTS diesel is a viable alternative energy pathway from LFG when compared to other pathways, primarily due to the main product being a renewable fuel that can serve as a drop-in fuel for diesel-based uses, within both the waste industry as well as the larger market. Further sensitivity analysis was performed based on the production of TriFTS diesel with the counterfactual waste management scenario of LFG-to-Flaring as well as the alternative LFG-to-Electricity waste management pathway. The sensitivity of the carbon intensity for TriFTS diesel to flaring efficiency and the carbon intensity of the electricity grid were also investigated. The study highlights the potential for the TriFTS conversion process technology to contribute to the waste industry's closed loop and decarbonization initiatives and to provide low carbon fuel for transportation.

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Mechanism of Cobalt-Catalyzed CO Hydrogenation: 2. Fischer-Tropsch Synthesis.

Publications

Mechanism of Cobalt-Catalyzed CO Hydrogenation: 2. Fischer-Tropsch Synthesis.

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