4.6 Article

Activity and deactivation of Ru supported on La1.6Sr0.4NiO4 perovskite-like catalysts prepared by different methods for decomposition of N2O

Journal

CATALYSIS SCIENCE & TECHNOLOGY
Volume 6, Issue 24, Pages 8505-8515

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/C6CY01920J

Keywords

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Funding

  1. Natural Sciences Fund of Heilongjiang Province [B2015009]
  2. Foundation of Educational Commission of Heilongjiang Province of China [11531286]
  3. Postdoctoral Science-research Developmental Foundation of Heilongjiang Province of China [LBH-Q12022]
  4. Innovative Research Project of Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education

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In this paper, the activity and stability of Ru supported on La1.6Sr0.4NiO4 perovskite-like catalysts prepared by two different methods, incipient wetness procedures with the addition of ethylene glycol (Ru/LSN-EG) and without ethylene glycol (Ru/LSN), were investigated for the decomposition of N2O. The catalysts were fully characterized by means of XRD, elemental analysis, N-2-physisorption, TEM, H-2-TPR, N2O-TPD and XPS. The Ru/LSN-EG catalyst retained high activity for 10 h without deactivation, which is attributed to the stable Ru3+ species, the much higher mobility of lattice oxygen and the regeneration ability of oxygen vacancies. However, the Ru/LSN catalyst presented deactivation; the initial N2O conversion of about 95% was only maintained for the first hour and decreased with time to 55% after 6 h. The reasons for this deactivation were investigated by a series of experiments and characterizations. The results indicate that the deactivation of the Ru/LSN catalyst can be ascribed to the difficult desorption of the oxygen species derived from N2O decomposition on the active sites; moreover, all the metallic Ru and Ru3+ species are oxidized to high oxidation state Ru4+ species. All the results demonstrated that the Ru3+ species was more favorable for N2O decomposition. Furthermore, the effects of O-2 and H2O on the decomposition of N2O were also evaluated over the Ru/LSN-EG catalyst. High stability and no irreversible deactivation of the Ru/LSN-EG catalyst, even in the presence of O-2 and H2O, were found.

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