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

Abstract

Methane is converted over nickel on ceria zirconia (Ni/CZ) to ethane, aromatics and hydrogen at steady state up to the thermodynamic limit at temperatures of 350 oC to 500 oC. At 450 oC and 500 oC, 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. In addition, 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. On these sites, surface species couple into higher alkyl chains, which can be desorbed as ethane. It is suggested that these Ni sites are too small to assemble aromatic deposits and hence, they remain active throughout the reaction.

Authors:
 [1];  [2];  [3];  [4];  [2]
  1. GEORGIA INSTITUTE OF TECH
  2. Georgia Institute of Technology
  3. BATTELLE (PACIFIC NW LAB)
  4. Brookhaven National Laboratory
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1514258
Report Number(s):
PNNL-SA-131737
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 10; Journal Issue: 12
Country of Publication:
United States
Language:
English

Citation Formats

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., 2018. 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. Thu . "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_1514258,
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) to ethane, aromatics and hydrogen at steady state up to the thermodynamic limit at temperatures of 350 oC to 500 oC. At 450 oC and 500 oC, 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. In addition, 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. On these sites, surface species couple into higher alkyl chains, which can be desorbed as ethane. 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 = {6}
}

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