4.7 Article

Effect of zirconia morphology on sulfur-resistant methanation performance of MoO3/ZrO2 catalyst

Journal

APPLIED SURFACE SCIENCE
Volume 441, Issue -, Pages 482-490

Publisher

ELSEVIER SCIENCE BV
DOI: 10.1016/j.apsusc.2018.02.019

Keywords

Sulfur-resistant methanation; Monoclinic ZrO2; Tetragonal ZrO2; MoS2

Funding

  1. National High Technology Research and Development Program of China [2015AA050504]
  2. National Natural Science Foundation of China [21576203, 21606167]

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Two kinds of ZrO2 support with different morphologies were prepared by facile solvothermal method in different solvents. The obtained two supports showed monoclinic zirconia (m-ZrO2) and tetragonal zirconia (t-ZrO2) phase with similar crystalline size. Their supported Mo-based catalysts were prepared by impregnation method and the effect of zirconia morphology on the performance of sulfur-resistant methanation was examined. The results indicated that the MoO3/m-ZrO2 has higher CO conversion than the MoO3/t-ZrO2 catalyst. Characterizations by XRD, Raman, H-2-TPR and IR confirmed that the m-ZrO2 is superior to t-ZrO2 for dispersing molybdenum species. In addition, the MoO3/m-ZrO2 catalyst has weaker interaction between support and active Mo speices than the MoO3/t-ZrO2 catalyst, which facilitates to forming active species of nanocrystalline MoS2 layers for sulfur-resistant methanation. The weaker interaction of molybdenum species with m-ZrO2 is related with the more covalent character of the Zr-O bond and more oxygen defective structure of m-ZrO2. A larger number of Lewis acid centers appear on the surface of m-ZrO2, which verified the substantial vacancies on m-ZrO2 exposing coordinately unsaturated Zr3+ and Zr4+ cations. Meanwhile, the less Lewis acid of t-ZrO2 result in stronger interaction between support and molybdenum species and trigger crystalline phase MoO3 and Mo-O-Zr linkages. (C) 2018 Elsevier B.V. All rights reserved.

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