Chinese Journal of Catalysis

Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (12): 2122-2133.DOI: 10.1016/S1872-2067(16)62540-8

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Morphology effect of zirconia support on the catalytic performance of supported Ni catalysts for dry reforming of methane

Weizuo Lia, Zhongkui Zhaoa, Yanhua Jiaob, Guiru Wanga   

  1. a State Key Laboratory of Fine Chemicals, Department of Catalysis Chemistry and Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China;
    b College of Material Chemistry and Chemical Engineering, Hangzhou Normal University, Hangzhou 310036, Zhejiang, China
  • Received:2016-08-29 Revised:2016-09-30 Online:2016-12-27 Published:2016-12-27
  • Contact: Zhongkui Zhao
  • Supported by:

    This work was financially supported by the Joint Fund of Coal, set up by National Natural Science Foundation of China and Shenhua Co., Ltd. (U1261104), the National Natural Science Foundation of China (21276041), the Program for New Century Excellent Talents in University (NCET-12-0079), the Natural Science Foundation of Liaoning Province (2015020200), the Fundamental Research Funds for the Central Universities (DUT15LK41), and the Science and Technology Development Program of Hangzhou (20130533B14).

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Abstract:

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, N2 adsorption measurement (BET), TEM, H2-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.

Key words: Ni-based catalyst, ZrO2 support, Hierarchical structure, Morphology effect, Dry reforming of methane, Synthesis gas, Coke resistance