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Confined small-sized cobalt catalysts stimulate carbon-chain growth reversely by modifying ASF law of Fischer-Tropsch synthesis.

ABSTRACT: Fischer-Tropsch synthesis (FTS) is a promising technology to convert syngas derived from non-petroleum-based resources to valuable chemicals or fuels. Selectively producing target products will bring great economic benefits, but unfortunately it is theoretically limited by Anderson-Schulz-Flory (ASF) law. Herein, we synthesize size-uniformed cobalt nanocrystals embedded into mesoporous SiO₂ supports, which is likely the structure of water-melon seeds inside pulps. We successfully tune the selectivity of products from diesel-range hydrocarbons (66.2%) to gasoline-range hydrocarbons (62.4%) by controlling the crystallite sizes of confined cobalt from 7.2 to 11.4?nm, and modify the ASF law. Generally, larger Co crystallites increase carbon-chain growth, producing heavier hydrocarbons. But here, we interestingly observe a reverse phenomenon: the uniformly small-sized cobalt crystallites can strongly adsorb active C* species, and the confined structure will inhibit aggregation of cobalt crystallites and escape of reaction intermediates in FTS, inducing the higher selectivity towards heavier hydrocarbons.

SUBMITTER: Cheng Q

PROVIDER: S-EPMC6092428 | biostudies-literature | 2018 Aug

REPOSITORIES: biostudies-literature

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Confined small-sized cobalt catalysts stimulate carbon-chain growth reversely by modifying ASF law of Fischer-Tropsch synthesis.

Cheng Qingpeng Q Tian Ye Y Lyu Shuaishuai S Zhao Na N Ma Kui K Ding Tong T Jiang Zheng Z Wang Lihua L Zhang Jing J Zheng Lirong L Gao Fei F Dong Lin L Tsubaki Noritatsu N Li Xingang X

Nature communications 20180814 1

Fischer-Tropsch synthesis (FTS) is a promising technology to convert syngas derived from non-petroleum-based resources to valuable chemicals or fuels. Selectively producing target products will bring great economic benefits, but unfortunately it is theoretically limited by Anderson-Schulz-Flory (ASF) law. Herein, we synthesize size-uniformed cobalt nanocrystals embedded into mesoporous SiO<sub>2</sub> supports, which is likely the structure of water-melon seeds inside pulps. We successfully tune ...[more]

PMID: 30108226

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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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Confined small-sized cobalt catalysts stimulate carbon-chain growth reversely by modifying ASF law of Fischer-Tropsch synthesis.

Publications

Confined small-sized cobalt catalysts stimulate carbon-chain growth reversely by modifying ASF law of Fischer-Tropsch synthesis.

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