Carbon Nanotube Formation on Cr-Doped Ferrite Catalyst during Water Gas Shift Membrane Reaction: Mechanistic Implications and Extended Studies on Dry Gas Conversions
Abstract
A nanocrystalline chromium-doped ferrite (FeCr) catalyst was shown to coproduce H2 and multiwalled carbon nanotubes (MWCNTs) during water gas shift (WGS) reaction in a H2-permselective zeolite membrane reactor (MR) at reaction pressures of ~20 bar. The FeCr catalyst was further demonstrated in the synthesis of highly crystalline and dimensionally uniform MWCNTs from a dry gas mixture of CO and CH4, which were the apparent sources for MWCNT growth in the WGS MR. In both the WGS MR and dry gas reactions, the operating temperature was 500 °C, which is significantly lower than those commonly used in MWCNT production by chemical vapor deposition (CVD) method from CO, CH4, or any other precursor gases. Extensive ex situ characterizations of the reaction products revealed that the FeCr catalyst remained in partially reduced states of Fe3+/Fe2+ and Cr6+/Cr3+ in WGS membrane reaction while further reduction of Fe2+ to Fe0 occurred in the CO/CH4 dry gas environments. The formation of the metallic Fe nanoparticles or catalyst surface dramatically improved the crystallinity and dimensional uniformity of the MWCNTs from dry gas reaction as compared to that from WGS reaction in the MR. Reaction of the CO/CH4 mixture containing 500 ppmv H2S also resulted in high-quality MWCNTsmore »
- Authors:
- Publication Date:
- Research Org.:
- Arizona State Univ., Tempe, AZ (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE); USDOE Office of Fossil Energy (FE)
- OSTI Identifier:
- 1647268
- Alternate Identifier(s):
- OSTI ID: 1799846
- Grant/Contract Number:
- FE0026435
- Resource Type:
- Published Article
- Journal Name:
- Catalysts
- Additional Journal Information:
- Journal Name: Catalysts Journal Volume: 10 Journal Issue: 8; Journal ID: ISSN 2073-4344
- Publisher:
- MDPI AG
- Country of Publication:
- Switzerland
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Cr-doped ferrite; membrane reactor; water gas shift; carbon nanotubes; sulfur resistance
Citation Formats
Sun, Xinhui, Arvanitis, Antonios, Damma, Devaiah, Alvarez, Noe T., Shanov, Vesselin, Smirniotis, Panagiotis G., and Dong, Junhang. Carbon Nanotube Formation on Cr-Doped Ferrite Catalyst during Water Gas Shift Membrane Reaction: Mechanistic Implications and Extended Studies on Dry Gas Conversions. Switzerland: N. p., 2020.
Web. doi:10.3390/catal10080927.
Sun, Xinhui, Arvanitis, Antonios, Damma, Devaiah, Alvarez, Noe T., Shanov, Vesselin, Smirniotis, Panagiotis G., & Dong, Junhang. Carbon Nanotube Formation on Cr-Doped Ferrite Catalyst during Water Gas Shift Membrane Reaction: Mechanistic Implications and Extended Studies on Dry Gas Conversions. Switzerland. https://doi.org/10.3390/catal10080927
Sun, Xinhui, Arvanitis, Antonios, Damma, Devaiah, Alvarez, Noe T., Shanov, Vesselin, Smirniotis, Panagiotis G., and Dong, Junhang. Wed .
"Carbon Nanotube Formation on Cr-Doped Ferrite Catalyst during Water Gas Shift Membrane Reaction: Mechanistic Implications and Extended Studies on Dry Gas Conversions". Switzerland. https://doi.org/10.3390/catal10080927.
@article{osti_1647268,
title = {Carbon Nanotube Formation on Cr-Doped Ferrite Catalyst during Water Gas Shift Membrane Reaction: Mechanistic Implications and Extended Studies on Dry Gas Conversions},
author = {Sun, Xinhui and Arvanitis, Antonios and Damma, Devaiah and Alvarez, Noe T. and Shanov, Vesselin and Smirniotis, Panagiotis G. and Dong, Junhang},
abstractNote = {A nanocrystalline chromium-doped ferrite (FeCr) catalyst was shown to coproduce H2 and multiwalled carbon nanotubes (MWCNTs) during water gas shift (WGS) reaction in a H2-permselective zeolite membrane reactor (MR) at reaction pressures of ~20 bar. The FeCr catalyst was further demonstrated in the synthesis of highly crystalline and dimensionally uniform MWCNTs from a dry gas mixture of CO and CH4, which were the apparent sources for MWCNT growth in the WGS MR. In both the WGS MR and dry gas reactions, the operating temperature was 500 °C, which is significantly lower than those commonly used in MWCNT production by chemical vapor deposition (CVD) method from CO, CH4, or any other precursor gases. Extensive ex situ characterizations of the reaction products revealed that the FeCr catalyst remained in partially reduced states of Fe3+/Fe2+ and Cr6+/Cr3+ in WGS membrane reaction while further reduction of Fe2+ to Fe0 occurred in the CO/CH4 dry gas environments. The formation of the metallic Fe nanoparticles or catalyst surface dramatically improved the crystallinity and dimensional uniformity of the MWCNTs from dry gas reaction as compared to that from WGS reaction in the MR. Reaction of the CO/CH4 mixture containing 500 ppmv H2S also resulted in high-quality MWCNTs similar to those from the H2S-free feed gas, demonstrating excellent sulfur tolerance of the FeCr catalyst that is practically meaningful for utilization of biogas and cheap coal-derived syngas.},
doi = {10.3390/catal10080927},
journal = {Catalysts},
number = 8,
volume = 10,
place = {Switzerland},
year = {Wed Aug 12 00:00:00 EDT 2020},
month = {Wed Aug 12 00:00:00 EDT 2020}
}
https://doi.org/10.3390/catal10080927
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