Abstract

The production of base chemicals such as olefins and aromatics from synthesis gas is of great interest from both an academic and an industrial point of view. We prepared a bulk iron Fischer Tropsch catalyst promoted with potassium capable of converting synthesis gas to olefins and combined it with an H-ZSM-5 zeolite to convert the formed olefins to aromatics on the zeolite acid sites. All experiments were performed in stacked bed mode to avoid migration of potassium promoters from the iron catalyst to the zeolite, which can deactivate acid sites in the zeolite. Operating at a pressure of 20 bar and temperatures between 250 °C and 300 °C instead of high temperatures of 300−350 °C led to a methane selectivity of only 7–14 %C. Olefins in the range of C4–C8 were converted to aromatics in the initial section of the zeolite bed, while further into the zeolite bed C2-C3 olefins oligomerized to longer olefins and alkylated light aromatics forming heavier aromatic hydrocarbons. Investigation of the influence of CO conversion on the aromatization of olefins showed a maximum in aromatic selectivity (excluding CO2) of 18 %C at medium CO conversion (XCO = 26–47 %). This work provides detailed insight into the chemical events that occur in bifunctional catalyst beds and can contribute to the development of an industrial process to convert synthesis gas to aromatics in a single reactor.

Highlights

  • To reduce the carbon footprint of chemical processes and the worldwide carbon dioxide emissions, new pathways for the production of chemicals need to be developed [1,2]

  • We investigated the influence of the zeolite bed height, and the residence time of olefins formed on the iron catalyst in the zeolite bed, in stacked bed

  • In this work we studied the influence of reaction conditions on the conversion of synthesis gas to aromatics with olefin intermediates by combining a potassium promoted bulk iron-based Fischer-Tropsch catalyst with an H-ZSM-5 zeolite in stacked bed mode in a single reactor

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Summary

Introduction

To reduce the carbon footprint of chemical processes and the worldwide carbon dioxide emissions, new pathways for the production of chemicals need to be developed [1,2]. Combining a sodium and sulfur promoted iron (carbide) FTO catalyst with the acid properties of a H-ZSM-5 zeolite in a high temperature and low pressure process (400 °C, 1 bar) resulted in the formation of C6-C8 aromatics with. We discuss a bulk iron catalyst promoted with potassium to convert synthesis gas to olefins at 250−300 °C and 20 bar, avoiding rapid deactivation and shifting the Anderson-Schulz-Flory distribution to higher alpha values by operating at relatively low temperatures. This results in an increase of average chain length of the hydrocarbon products.

Catalyst preparation
Catalyst characterization
Catalytic performance
Characterization
Influence of reaction temperature on the performance of the iron catalyst
Spent catalyst analysis
Conclusion

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