4.6 Article

Nanostructured Ce0.7Mn0.3O2-δ and Ce0.7Fe0.3O2-δ solid solutions for diesel soot oxidation

Journal

APPLIED CATALYSIS A-GENERAL
Volume 488, Issue -, Pages 1-10

Publisher

ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcata.2014.09.014

Keywords

Solid solution; Oxygen vacancies; Synergistic effect; Soot oxidation; Low temperature reducibility

Funding

  1. Council of Scientific and Industrial Research (CSIR), New Delhi
  2. Department of Science and Technology, New Delhi, under SERB [SB/S1/PC-106/2012]

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Nanostructured Ce0.7Mn0.3O2-delta (CM) and Ce0.7Fe0.3,O2-delta (CF) solid solutions were prepared by a facile coprecipitation method and evaluated for soot oxidation. The structural, morphological, and surface properties were investigated by various techniques, namely, XRD, ICP-OES, BET surface area, SEM-EDX, TEM-HRTEM, UV-vis DRS, Raman, FT-IR, XPS, H-2-TPR, and TGA-DTA. XRD and TEM results confirmed formation of nanocrystalline solid solutions with the incorporated Mn and/or Fe cations in the ceria lattice. SEM studies ensured nanoparticle nature of Ce-Mn-O and Ce-Fe-O solid solutions with homogeneous distribution. ICP-OES and EDX analysis confirmed actual amount of metal loadings in the respective catalysts. UV-vis DRS and Raman results revealed the formation of more oxygen vacancies, which lead to the creation of more surface active species (Ce4+/Ce3+ and O*). XPS results revealed that the doping of Mn and/or Fe into the ceria lattice makes some Ce4+ transferred into Ce3+ in order to maintain the electrical neutrality, thereby facilitate the reduction of Ce4+ --> Ce3+ and the formation of oxygen vacancies. TPR results showed that the mixed oxides reduce at lower temperatures than pure ceria. This observation confirmed that there is a synergetic interaction between Ce-O and M-O (M = Mn, Fe). The catalytic activity of CM and CF samples towards soot oxidation has been evaluated under tight contact conditions and compared with the well-established CeO2-ZrO2 (CZ) catalyst. Among the investigated catalysts, the Mn and/or Fe doped ceria solid solutions showed improved catalytic activity. The order of activity is as follows: CM > CF > CZ > C. Further, the CM and CF catalysts were found to be thermally quite stable compared to pure ceria. In particular, the CM sample exhibited superior catalytic activity (T-50 = similar to 665 K) and thermal stability towards soot oxidation. (C) 2014 Elsevier B.V. All rights reserved.

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