New mechanism insight for the hydrogenation of CO/CO2 gas mixtures to hydrocarbons over iron-based catalyst

Sandeep Badoga; Michela Martinelli; Muthu Kumaran Gnanamani; Young Koh; Wilson D. Shafer

doi:10.1016/j.catcom.2021.106284

New mechanism insight for the hydrogenation of CO/CO₂ gas mixtures to hydrocarbons over iron-based catalyst

Sandeep Badoga, Michela Martinelli, Muthu Kumaran Gnanamani, Young Koh, Wilson D. Shafer

Center for Applied Energy Research (CAER)

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

Iron-based catalysts are the most suitable candidates for converting CO₂ or CO₂-rich syngas to hydrocarbons. However, several issues about the mechanism of CO₂ hydrogenation are still unclear. In this work, we investigated the performance of an iron-based catalyst with H₂/CO₂, H₂/CO/N₂ and H₂/CO/¹³CO₂/N₂ gas mixtures at the same process conditions (T = 270°C, P = 175 psi and SV = 3 NL/h/g_cat). The CO₂ hydrogenation rate was much lower than that observed for CO hydrogenation. ¹³CO₂ tracer experiments indicated that CO₂ is hydrogenated to hydrocarbons via the reverse water-gas shift even when present in small concentration (1.8 vol%). ¹³C enrichment was observed in both CO and C₁-C₄ hydrocarbons.

Original language	English
Article number	106284
Journal	Catalysis Communications
Volume	152
DOIs	https://doi.org/10.1016/j.catcom.2021.106284
State	Published - Apr 2021

Bibliographical note

Publisher Copyright:
© 2021 The Author(s)

Keywords

C-labelled CO
CO hydrogenation
CO-rich syngas
Fischer-Tropsch
FTS mechanism
Iron catalyst

ASJC Scopus subject areas

Catalysis
General Chemistry
Process Chemistry and Technology

Access to Document

10.1016/j.catcom.2021.106284

Cite this

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title = "New mechanism insight for the hydrogenation of CO/CO2 gas mixtures to hydrocarbons over iron-based catalyst",

abstract = "Iron-based catalysts are the most suitable candidates for converting CO2 or CO2-rich syngas to hydrocarbons. However, several issues about the mechanism of CO2 hydrogenation are still unclear. In this work, we investigated the performance of an iron-based catalyst with H2/CO2, H2/CO/N2 and H2/CO/13CO2/N2 gas mixtures at the same process conditions (T = 270°C, P = 175 psi and SV = 3 NL/h/gcat). The CO2 hydrogenation rate was much lower than that observed for CO hydrogenation. 13CO2 tracer experiments indicated that CO2 is hydrogenated to hydrocarbons via the reverse water-gas shift even when present in small concentration (1.8 vol%). 13C enrichment was observed in both CO and C1-C4 hydrocarbons.",

keywords = "C-labelled CO, CO hydrogenation, CO-rich syngas, Fischer-Tropsch, FTS mechanism, Iron catalyst",

author = "Sandeep Badoga and Michela Martinelli and Gnanamani, {Muthu Kumaran} and Young Koh and Shafer, {Wilson D.}",

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AU - Badoga, Sandeep

AU - Martinelli, Michela

AU - Gnanamani, Muthu Kumaran

AU - Koh, Young

AU - Shafer, Wilson D.

PY - 2021/4

Y1 - 2021/4

N2 - Iron-based catalysts are the most suitable candidates for converting CO2 or CO2-rich syngas to hydrocarbons. However, several issues about the mechanism of CO2 hydrogenation are still unclear. In this work, we investigated the performance of an iron-based catalyst with H2/CO2, H2/CO/N2 and H2/CO/13CO2/N2 gas mixtures at the same process conditions (T = 270°C, P = 175 psi and SV = 3 NL/h/gcat). The CO2 hydrogenation rate was much lower than that observed for CO hydrogenation. 13CO2 tracer experiments indicated that CO2 is hydrogenated to hydrocarbons via the reverse water-gas shift even when present in small concentration (1.8 vol%). 13C enrichment was observed in both CO and C1-C4 hydrocarbons.

AB - Iron-based catalysts are the most suitable candidates for converting CO2 or CO2-rich syngas to hydrocarbons. However, several issues about the mechanism of CO2 hydrogenation are still unclear. In this work, we investigated the performance of an iron-based catalyst with H2/CO2, H2/CO/N2 and H2/CO/13CO2/N2 gas mixtures at the same process conditions (T = 270°C, P = 175 psi and SV = 3 NL/h/gcat). The CO2 hydrogenation rate was much lower than that observed for CO hydrogenation. 13CO2 tracer experiments indicated that CO2 is hydrogenated to hydrocarbons via the reverse water-gas shift even when present in small concentration (1.8 vol%). 13C enrichment was observed in both CO and C1-C4 hydrocarbons.

KW - C-labelled CO

KW - CO hydrogenation

KW - CO-rich syngas

KW - Fischer-Tropsch

KW - FTS mechanism

KW - Iron catalyst

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