4.7 Article

Lanthanide oxide modified nickel supported on mesoporous silica catalysts for dry reforming of methane

Journal

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
Volume 46, Issue 62, Pages 31608-31622

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2021.07.056

Keywords

Dry reforming of methane; Nickel catalysts; Lanthanide oxides; Kinetic study; Carbon deposition

Funding

  1. National Natural Science Foundation of China [21673079, 21872056]
  2. Natural Science Foundation of Guangdong Province [2021A1515010149]
  3. Guangzhou Municipal Science and Technology Project [20180410116]
  4. Science and Technology Planning Project of Guangdong Province [2015A020216002]

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In the dry reforming of methane reaction, the addition of lanthanide oxides significantly improves the carbon resistance of nickel-based catalysts, with NiLa/SiO2 and NiCe/SiO2 exhibiting better stability and catalytic activity. The presence of lanthanide oxides affects the size of Ni nanoparticles and the activation energy of methane and carbon dioxide dissociation, leading to enhanced carbon resistance and stability in NiLa/SiO2 and NiCe/SiO2 catalysts.
Addition of rare earth oxide, especially lanthanide oxide, was regarded as a promising strategy to improve the carbon resistance for Nickel-based catalysts in dry reforming of methane (DRM). In this work, Nickel-based catalysts containing lanthanide oxides (NiLa/SiO2, NiCe/SiO2, NiSm/SiO2, and NiGd/SiO2) were prepared and employed to catalyze DRM. Lanthanide oxide affected the formation of Ni nanoparticles in different size. In NiLa/SiO2 and NiCe/SiO2, Ni nanoparticles maintained relatively small size (4 nm), while in NiSm/SiO2 and NiGd/SiO2, nickel particles were in large size (8 nm). NiLa/SiO2 and NiCe/SiO2 exhibited better stability than the other two catalysts, with CH4 conversion decreasing from 64.6 to 57.6% and 61.6 to 60.3%, respectively in 10 h on stream. The kinetic study confirmed that adding lanthanide oxide significantly affected the activation energy of CH4 dissociation and CO2 dissociation. Compared to monometallic Ni/SiO2, the presence of Sm and Gd suppressed CO2 dissociation, and introduction of Ce and La effectively promoted CO2 dissociation. These characters contributed to the higher carbon resistance and good stability for NiLa/SiO2 and NiCe/SiO2 catalysts in DRM reaction. (C) 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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