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Structure sensitivity and its effect on methane turnover and carbon co-product selectivity in thermocatalytic decomposition of methane over supported Ni catalysts

Journal Article · · Applied Catalysis. A, General
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  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. West Virginia Univ., Morgantown, WV (United States)
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We explore how thermocatalytic decomposition of methane (TCD) is a promising approach for producing CO2-free hydrogen and solid carbon co-product. In this study, a series of Al2O3- and MgAl2O4-based Ni catalysts, prepared with varying synthesis and pretreatment methods, were evaluated for methane TCD performance at 650°C and characterized before and after reaction to elucidate activity-structure relationships. We found that methane TCD turnover increases with Ni particle size. Further, large Ni particle sizes (i.e., >20 nm) are selective toward the formation of carbon nanotubes (CNTs), while small Ni particle sizes (i.e., <10 nm) are selective toward the formation of graphitic carbon layers. The formation of graphitic carbon layers block access to Ni active sites, thus rendering the catalyst inactive more quickly than when CNTs are produced. Additionally, the catalyst deactivation observed with time-on-stream is due to the fragmentation of Ni particles into smaller Ni particles followed by their encapsulation with graphitic carbon layers.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1755019
Alternate ID(s):
OSTI ID: 1778323
Report Number(s):
PNNL-SA-158733
Journal Information:
Applied Catalysis. A, General, Journal Name: Applied Catalysis. A, General Vol. 611; ISSN 0926-860X
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Carbon nanotubes
Ni catalysts
Ni particle size
Structure sensitivity
Thermocatalytic decomposition