Journal
CHINESE JOURNAL OF CATALYSIS
Volume 37, Issue 12, Pages 2122-2133Publisher
SCIENCE PRESS
DOI: 10.1016/s1872-2067(16)62540-8
Keywords
Ni-based catalyst; ZrO2 support; Hierarchical structure; Morphology effect; Dry reforming of methane; Synthesis gas; Coke resistance
Funding
- National Natural Science Foundation of China [U1261104, 21276041]
- Shenhua Co., Ltd. [U1261104]
- Program for New Century Excellent Talents in University [NCET-12-0079]
- Natural Science Foundation of Liaoning Province [2015020200]
- Fundamental Research Funds for the Central Universities [DUT15LK41]
- Science and Technology Development Program of Hangzhou [20130533B14]
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An immature pinecone shaped hierarchically structured zirconia (ZrO2-ipch) and a cobblestone-like zirconia nanoparticulate (ZrO2-cs), both with the monoclinic phase (m-phase), were synthesized by the facile hydrothermal method and used as the support for a Ni catalyst for the dry reforming of methane (DRM) with CO2. ZrO2-ipch is a much better support than ZrO2-cs and the traditional ZrO2 irregular particles made by a simple precipitation method (ZrO2-ip). The supported Ni catalyst on ZrO2-ipch (Ni/ZrO2-ipch) exhibited outstanding catalytic activity and coke-resistant stability compared to the ones on ZrO2-cs (Ni/ZrO2-cs) and ZrO2-ip (Ni/ZrO2-ip). Ni/ZrO2-ip exhibited the worst catalytic performance. The origin of the significantly enhanced catalytic performance was revealed by characterization including XRD, N-2 adsorption measurement (BET), TEM, H-2-TPR, CO chemisorption, CO2-TPD, XPS and TGA. The superior catalytic activity of Ni/ZrO2-ipch to Ni/ZrO2-cs or Ni/ZrO2-ip was ascribed to a higher Ni dispersion, increased reducibility, enhanced oxygen mobility, and more basic sites with a higher strength, which were due to the unique hierarchically structural morphology of the ZrO2-ipch support. Ni/ZrO2-ipch exhibited better stability for the DRM reaction than Ni/ZrO2-ip, which was ascribed to its higher resistance to Ni sintering due to a strengthened metal-support interaction and the confinement effect of the mesopores and coke deposition resistance. The higher coking resistance of Ni/ZrO2-ipch for the DRM reaction in comparison with Ni/ZrO2-ip orignated from the coke-removalability of the higher amount of lattice oxygen and more basic sites, confirmed by XPS and CO2-TPD analysis, and the stabilized Ni on the Ni/ZrO2-ipch catalyst by the confinement effect of the mesopores of the hierarchical ZrO2-ipch support. The superior catalytic performance and coking resistance of the Ni/ZrO2-ipch catalyst makes it a promising candidate for synthesis gas production from the DRM reaction. (C) 2016, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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