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Title: Catalytic Nonoxidation Dehydrogenation of Ethane Over Fe-Ni Catalysts Supported on Mg (Al)O to Produce Hydrogen and Easily Purified Carbon Nanotubes

Abstract

Nonoxidative decomposition of ethane was conducted over monometallic Ni and bimetallic Fe-Ni catalysts on basic Mg(Al)O support to produce H2 free of CO and CO2 and easily purified carbon nanotubes, a potentially valuable byproduct. The Mg(Al)O support was prepared by calcination of synthetic MgAl-hydrotalcite with a Mg to Al ratio of 5. The catalysts were prepared by incipient wetness with total metal loadings of 5 wt %. The dehydrogenation of undiluted ethane was conducted at temperatures of 500, 650, and 700 C. At 500 C, the Ni/Mg(Al)O catalyst was highly active and very stable with 100% conversion of ethane to 20 vol % H2 and 80 vol % CH4. However, the bimetallic Fe-Ni/Mg(Al)O exhibited its best performance at 650 C, yielding 65 vol % H2, 10 vol % CH4, and 25 vol % unreacted ethane. The product carbon was in the form of carbon nanotubes (CNT) at all three reaction temperatures, but the morphology of the CNT depended on both the catalyst composition and reaction temperature. The CNTs were formed by a tip-growth mechanism over the Mg(Al)O supported catalysts and were easily purified by a one-step dilute nitric acid treatment. Mossbauer spectroscopy, X-ray absorption fine structure spectroscopy, N2 adsorption-desorption isotherms,more » TEM, STEM, TGA, and XRD were used to characterize the catalysts and the CNT, revealing the catalytic mechanisms.« less

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Org.:
Doe - Office Of Science
OSTI Identifier:
960049
Report Number(s):
BNL-83035-2009-JA
Journal ID: ISSN 0887-0624; ENFUEM; TRN: US201016%%1193
DOE Contract Number:  
DE-AC02-98CH10886
Resource Type:
Journal Article
Journal Name:
Energy and Fuels
Additional Journal Information:
Journal Volume: 21; Journal Issue: 6; Journal ID: ISSN 0887-0624
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; ABSORPTION; CALCINATION; CARBON; CATALYSTS; DEHYDROGENATION; ETHANE; FINE STRUCTURE; HYDROGEN; ISOTHERMS; MORPHOLOGY; NANOTUBES; NITRIC ACID; PERFORMANCE; SPECTROSCOPY; X-RAY DIFFRACTION; national synchrotron light source

Citation Formats

Shen, W, Wang, Y, Shi, X, Shah, N, Huggins, F, Bollineni, S, Seehra, M, and Huffman, G. Catalytic Nonoxidation Dehydrogenation of Ethane Over Fe-Ni Catalysts Supported on Mg (Al)O to Produce Hydrogen and Easily Purified Carbon Nanotubes. United States: N. p., 2007. Web. doi:10.1021/ef7004018.
Shen, W, Wang, Y, Shi, X, Shah, N, Huggins, F, Bollineni, S, Seehra, M, & Huffman, G. Catalytic Nonoxidation Dehydrogenation of Ethane Over Fe-Ni Catalysts Supported on Mg (Al)O to Produce Hydrogen and Easily Purified Carbon Nanotubes. United States. doi:10.1021/ef7004018.
Shen, W, Wang, Y, Shi, X, Shah, N, Huggins, F, Bollineni, S, Seehra, M, and Huffman, G. Mon . "Catalytic Nonoxidation Dehydrogenation of Ethane Over Fe-Ni Catalysts Supported on Mg (Al)O to Produce Hydrogen and Easily Purified Carbon Nanotubes". United States. doi:10.1021/ef7004018.
@article{osti_960049,
title = {Catalytic Nonoxidation Dehydrogenation of Ethane Over Fe-Ni Catalysts Supported on Mg (Al)O to Produce Hydrogen and Easily Purified Carbon Nanotubes},
author = {Shen, W and Wang, Y and Shi, X and Shah, N and Huggins, F and Bollineni, S and Seehra, M and Huffman, G},
abstractNote = {Nonoxidative decomposition of ethane was conducted over monometallic Ni and bimetallic Fe-Ni catalysts on basic Mg(Al)O support to produce H2 free of CO and CO2 and easily purified carbon nanotubes, a potentially valuable byproduct. The Mg(Al)O support was prepared by calcination of synthetic MgAl-hydrotalcite with a Mg to Al ratio of 5. The catalysts were prepared by incipient wetness with total metal loadings of 5 wt %. The dehydrogenation of undiluted ethane was conducted at temperatures of 500, 650, and 700 C. At 500 C, the Ni/Mg(Al)O catalyst was highly active and very stable with 100% conversion of ethane to 20 vol % H2 and 80 vol % CH4. However, the bimetallic Fe-Ni/Mg(Al)O exhibited its best performance at 650 C, yielding 65 vol % H2, 10 vol % CH4, and 25 vol % unreacted ethane. The product carbon was in the form of carbon nanotubes (CNT) at all three reaction temperatures, but the morphology of the CNT depended on both the catalyst composition and reaction temperature. The CNTs were formed by a tip-growth mechanism over the Mg(Al)O supported catalysts and were easily purified by a one-step dilute nitric acid treatment. Mossbauer spectroscopy, X-ray absorption fine structure spectroscopy, N2 adsorption-desorption isotherms, TEM, STEM, TGA, and XRD were used to characterize the catalysts and the CNT, revealing the catalytic mechanisms.},
doi = {10.1021/ef7004018},
journal = {Energy and Fuels},
issn = {0887-0624},
number = 6,
volume = 21,
place = {United States},
year = {2007},
month = {1}
}