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Title: Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures

Methane is converted over nickel on ceria zirconia (Ni/CZ) into ethane, aromatics, and hydrogen at steady state up to the thermodynamic limit at temperatures of 350 to 500 °C. At 450 and 500 °C, traces of ethylene are also produced. Ni/NiO particles activate methane and couple the resulting surface species to hydrocarbon products. Large Ni particles are responsible for the formation of carbonaceous deposits. Furthermore, aromatics are formed on these sites. Smaller Ni/NiO particles are responsible for the formation of ethane and ethylene and appear to provide sustained activity. It is suggested that these Ni sites are too small to assemble aromatic deposits, and hence they remain active throughout the reaction.
Authors:
 [1] ;  [1] ;  [2] ;  [2] ; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Publication Date:
Report Number(s):
BNL-209099-2018-JAAM
Journal ID: ISSN 1867-3880
Grant/Contract Number:
SC0012704; SC0016486; AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 10; Journal Issue: 12; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; carbon nanotubes; coking dispersion; Lewis acids; nickel oxide
OSTI Identifier:
1475145
Alternate Identifier(s):
OSTI ID: 1437199

Okolie, Chukwuemeka, Lyu, Yimeng, Kovarik, Libor, Stavitski, Eli, and Sievers, Carsten. Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures. United States: N. p., Web. doi:10.1002/cctc.201701892.
Okolie, Chukwuemeka, Lyu, Yimeng, Kovarik, Libor, Stavitski, Eli, & Sievers, Carsten. Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures. United States. doi:10.1002/cctc.201701892.
Okolie, Chukwuemeka, Lyu, Yimeng, Kovarik, Libor, Stavitski, Eli, and Sievers, Carsten. 2018. "Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures". United States. doi:10.1002/cctc.201701892.
@article{osti_1475145,
title = {Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures},
author = {Okolie, Chukwuemeka and Lyu, Yimeng and Kovarik, Libor and Stavitski, Eli and Sievers, Carsten},
abstractNote = {Methane is converted over nickel on ceria zirconia (Ni/CZ) into ethane, aromatics, and hydrogen at steady state up to the thermodynamic limit at temperatures of 350 to 500 °C. At 450 and 500 °C, traces of ethylene are also produced. Ni/NiO particles activate methane and couple the resulting surface species to hydrocarbon products. Large Ni particles are responsible for the formation of carbonaceous deposits. Furthermore, aromatics are formed on these sites. Smaller Ni/NiO particles are responsible for the formation of ethane and ethylene and appear to provide sustained activity. It is suggested that these Ni sites are too small to assemble aromatic deposits, and hence they remain active throughout the reaction.},
doi = {10.1002/cctc.201701892},
journal = {ChemCatChem},
number = 12,
volume = 10,
place = {United States},
year = {2018},
month = {1}
}

Works referenced in this record:

Adsorption of Gases in Multimolecular Layers
journal, February 1938
  • Brunauer, Stephen; Emmett, P. H.; Teller, Edward
  • Journal of the American Chemical Society, Vol. 60, Issue 2, p. 309-319
  • DOI: 10.1021/ja01269a023