Fischer-Tropsch synthesis: Effect of Cu, Mn and Zn addition on activity and product selectivity of cobalt ferrite

Muthu Kumaran Gnanamani; Hussein H. Hamdeh; Gary Jacobs; Dali Qian; Fang Liu; Shelley D. Hopps; Gerald A. Thomas; Wilson D. Shafer; Qunfeng Xiao; Yongfeng Hu; Burtron H. Davis

doi:10.1039/c6ra10150j

Fischer-Tropsch synthesis: Effect of Cu, Mn and Zn addition on activity and product selectivity of cobalt ferrite

Muthu Kumaran Gnanamani, Hussein H. Hamdeh, Gary Jacobs, Dali Qian, Fang Liu, Shelley D. Hopps, Gerald A. Thomas, Wilson D. Shafer, Qunfeng Xiao, Yongfeng Hu, Burtron H. Davis

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Abstract

The effect of Cu, Mn and Zn addition on cobalt ferrite was investigated for Fischer-Tropsch synthesis (FTS). Oxalate co-precipitation followed by decomposition under inert conditions was used to obtain various metal containing cobalt ferrites (Co_0.7M_0.3Fe₂O₄). The carburization of cobalt ferrite in flowing CO at 270 °C and 175 psig yielded iron carbides (χ-Fe₅C₂ and ϵ′-Fe_2.2C) along with a bimetallic FeCo alloy. The extent of carburization was compared among Cu, Mn, and Zn doped catalysts with undoped cobalt ferrites under similar conditions. XRD and Mössbauer spectroscopy analysis of the freshly carburized samples followed by passivation revealed that carburization of cobalt ferrite did not change appreciably with addition of Cu or Mn. On the other hand, Zn was found to retard the carburization of cobalt ferrite. Analysis of the used FT catalysts suggests that Cu is less efficient over Mn and Zn in stabilizing the iron carbides (i.e., active form of iron) during FT synthesis. The FT activity remains more or less the same for the undoped, Cu and Zn containing cobalt ferrites at higher temperatures. The CO conversion of Co_0.7Mn_0.3Fe_2.0 catalyst was much lower than the other catalysts tested. Addition of Zn or Mn to cobalt ferrite was found to promote alcohol formation, particularly at higher reaction temperatures. The water-gas shift activity of the catalysts was found to decrease in the following order, Co_1.0Fe_2.0 > Co_0.7Mn_0.3Fe_2.0 > Co_0.7Zn_0.3Fe_2.0 > Co_0.7Cu_0.3Fe_2.0.

Original language	English
Pages (from-to)	62356-62367
Number of pages	12
Journal	RSC Advances
Volume	6
Issue number	67
DOIs	https://doi.org/10.1039/c6ra10150j
State	Published - 2016

Bibliographical note

Funding Information:
This work carried out at the CAER was supported by the Commonwealth of Kentucky. Research described in this paper was performed in part at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, the Natural Sciences and Engineering Research Council of Canada, the National Research Council Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan.

Publisher Copyright:
© 2016 The Royal Society of Chemistry.

Funding

This work carried out at the CAER was supported by the Commonwealth of Kentucky. Research described in this paper was performed in part at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, the Natural Sciences and Engineering Research Council of Canada, the National Research Council Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan.

Funders	Funder number
Government of Saskatchewan
University of Saskatchewan
Canadian Institutes of Health Research
Natural Sciences and Engineering Research Council of Canada
Western Economic Diversification Canada
National Research Council Canada (NRCC)
Canada Foundation for Innovation

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering

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@article{50df0bb59d864a0faacdcea7326b6484,

title = "Fischer-Tropsch synthesis: Effect of Cu, Mn and Zn addition on activity and product selectivity of cobalt ferrite",

abstract = "The effect of Cu, Mn and Zn addition on cobalt ferrite was investigated for Fischer-Tropsch synthesis (FTS). Oxalate co-precipitation followed by decomposition under inert conditions was used to obtain various metal containing cobalt ferrites (Co0.7M0.3Fe2O4). The carburization of cobalt ferrite in flowing CO at 270 °C and 175 psig yielded iron carbides (χ-Fe5C2 and ϵ′-Fe2.2C) along with a bimetallic FeCo alloy. The extent of carburization was compared among Cu, Mn, and Zn doped catalysts with undoped cobalt ferrites under similar conditions. XRD and M{\"o}ssbauer spectroscopy analysis of the freshly carburized samples followed by passivation revealed that carburization of cobalt ferrite did not change appreciably with addition of Cu or Mn. On the other hand, Zn was found to retard the carburization of cobalt ferrite. Analysis of the used FT catalysts suggests that Cu is less efficient over Mn and Zn in stabilizing the iron carbides (i.e., active form of iron) during FT synthesis. The FT activity remains more or less the same for the undoped, Cu and Zn containing cobalt ferrites at higher temperatures. The CO conversion of Co0.7Mn0.3Fe2.0 catalyst was much lower than the other catalysts tested. Addition of Zn or Mn to cobalt ferrite was found to promote alcohol formation, particularly at higher reaction temperatures. The water-gas shift activity of the catalysts was found to decrease in the following order, Co1.0Fe2.0 > Co0.7Mn0.3Fe2.0 > Co0.7Zn0.3Fe2.0 > Co0.7Cu0.3Fe2.0.",

author = "Gnanamani, {Muthu Kumaran} and Hamdeh, {Hussein H.} and Gary Jacobs and Dali Qian and Fang Liu and Hopps, {Shelley D.} and Thomas, {Gerald A.} and Shafer, {Wilson D.} and Qunfeng Xiao and Yongfeng Hu and Davis, {Burtron H.}",

note = "Funding Information: This work carried out at the CAER was supported by the Commonwealth of Kentucky. Research described in this paper was performed in part at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, the Natural Sciences and Engineering Research Council of Canada, the National Research Council Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. Publisher Copyright: {\textcopyright} 2016 The Royal Society of Chemistry.",

year = "2016",

doi = "10.1039/c6ra10150j",

language = "English",

volume = "6",

pages = "62356--62367",

number = "67",

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TY - JOUR

T1 - Fischer-Tropsch synthesis

T2 - Effect of Cu, Mn and Zn addition on activity and product selectivity of cobalt ferrite

AU - Gnanamani, Muthu Kumaran

AU - Hamdeh, Hussein H.

AU - Jacobs, Gary

AU - Qian, Dali

AU - Liu, Fang

AU - Hopps, Shelley D.

AU - Thomas, Gerald A.

AU - Shafer, Wilson D.

AU - Xiao, Qunfeng

AU - Hu, Yongfeng

AU - Davis, Burtron H.

N1 - Funding Information: This work carried out at the CAER was supported by the Commonwealth of Kentucky. Research described in this paper was performed in part at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, the Natural Sciences and Engineering Research Council of Canada, the National Research Council Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. Publisher Copyright: © 2016 The Royal Society of Chemistry.

PY - 2016

Y1 - 2016

N2 - The effect of Cu, Mn and Zn addition on cobalt ferrite was investigated for Fischer-Tropsch synthesis (FTS). Oxalate co-precipitation followed by decomposition under inert conditions was used to obtain various metal containing cobalt ferrites (Co0.7M0.3Fe2O4). The carburization of cobalt ferrite in flowing CO at 270 °C and 175 psig yielded iron carbides (χ-Fe5C2 and ϵ′-Fe2.2C) along with a bimetallic FeCo alloy. The extent of carburization was compared among Cu, Mn, and Zn doped catalysts with undoped cobalt ferrites under similar conditions. XRD and Mössbauer spectroscopy analysis of the freshly carburized samples followed by passivation revealed that carburization of cobalt ferrite did not change appreciably with addition of Cu or Mn. On the other hand, Zn was found to retard the carburization of cobalt ferrite. Analysis of the used FT catalysts suggests that Cu is less efficient over Mn and Zn in stabilizing the iron carbides (i.e., active form of iron) during FT synthesis. The FT activity remains more or less the same for the undoped, Cu and Zn containing cobalt ferrites at higher temperatures. The CO conversion of Co0.7Mn0.3Fe2.0 catalyst was much lower than the other catalysts tested. Addition of Zn or Mn to cobalt ferrite was found to promote alcohol formation, particularly at higher reaction temperatures. The water-gas shift activity of the catalysts was found to decrease in the following order, Co1.0Fe2.0 > Co0.7Mn0.3Fe2.0 > Co0.7Zn0.3Fe2.0 > Co0.7Cu0.3Fe2.0.

AB - The effect of Cu, Mn and Zn addition on cobalt ferrite was investigated for Fischer-Tropsch synthesis (FTS). Oxalate co-precipitation followed by decomposition under inert conditions was used to obtain various metal containing cobalt ferrites (Co0.7M0.3Fe2O4). The carburization of cobalt ferrite in flowing CO at 270 °C and 175 psig yielded iron carbides (χ-Fe5C2 and ϵ′-Fe2.2C) along with a bimetallic FeCo alloy. The extent of carburization was compared among Cu, Mn, and Zn doped catalysts with undoped cobalt ferrites under similar conditions. XRD and Mössbauer spectroscopy analysis of the freshly carburized samples followed by passivation revealed that carburization of cobalt ferrite did not change appreciably with addition of Cu or Mn. On the other hand, Zn was found to retard the carburization of cobalt ferrite. Analysis of the used FT catalysts suggests that Cu is less efficient over Mn and Zn in stabilizing the iron carbides (i.e., active form of iron) during FT synthesis. The FT activity remains more or less the same for the undoped, Cu and Zn containing cobalt ferrites at higher temperatures. The CO conversion of Co0.7Mn0.3Fe2.0 catalyst was much lower than the other catalysts tested. Addition of Zn or Mn to cobalt ferrite was found to promote alcohol formation, particularly at higher reaction temperatures. The water-gas shift activity of the catalysts was found to decrease in the following order, Co1.0Fe2.0 > Co0.7Mn0.3Fe2.0 > Co0.7Zn0.3Fe2.0 > Co0.7Cu0.3Fe2.0.

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ER -

Fischer-Tropsch synthesis: Effect of Cu, Mn and Zn addition on activity and product selectivity of cobalt ferrite

Abstract

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