Modification of Mn-Fe mixed oxide catalysts for low-temperature NH3-SCR of NO from marine diesel exhausts
A series of Mn-Fe mixed oxides doped with CeO2, Al2O3 and Sm2O3 were prepared by a simple coprecipitation method and applied as NH3-SCR catalysts to treat the NO of marine diesel exhausts. The effects of these promoters on the structural properties of Mn-Fe oxides were investigated by XRD, BET, SEM,...
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Veröffentlicht in: | Journal of environmental chemical engineering 2022-06, Vol.10 (3), p.107772, Article 107772 |
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Sprache: | eng |
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Zusammenfassung: | A series of Mn-Fe mixed oxides doped with CeO2, Al2O3 and Sm2O3 were prepared by a simple coprecipitation method and applied as NH3-SCR catalysts to treat the NO of marine diesel exhausts. The effects of these promoters on the structural properties of Mn-Fe oxides were investigated by XRD, BET, SEM, FT-IR, TG, TPR, TPD and XPS techniques. The results of catalytic tests showed that the Mn-Fe oxide catalyst co-doped with CeO2, Al2O3 and Sm2O3 exhibited the best deNOx activity and SO2 tolerance. The XRD, BET and SEM results revealed that the addition of Ce promoted the formation of Mn-Fe solid solutions and the introduction of Al enhanced the dispersion of different elements in the catalysts. The H2-TPR and NH3-TPD results suggested that the reduction properties were adjusted to a good balance and the surface acidity sites greatly increased by the addition of Ce, Al, and Sm species, which were in agreement with the improvement of the catalytic activity below 240 ℃. In addition, the XPS spectra indicated that the high concentrations of Fe3+and Mn3+ in surfaces of catalysts modified with Al and Sm could significantly enhance the redox catalytic cycles owing to the electronic transfer between them, and the Sm doping could simultaneously raise the fraction of Ce3+ by the reduction of Mn4+ and Ce4+ and thus suppress SO2 poisoning owing to the electron transfer between M4+ and SO2, which were contributed to the improvement of activity and SO2 resistance of mixed oxide catalysts.
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•Manganese-iron mixed oxides modified with Ce, Al and/or Sm were prepared as NH3-SCR catalysts for Marine diesel emissions.•Mn-Fe oxide catalysts co-doped by Ce, Al and Sm maintained 94% NO conversion under 10 vol% H2O and150 ppm SO2 at 225 ℃.•Superioractivity and SO2-resistance attributed to the electronic transfer between high concentrations of Mn3+ and Fe3+.•Ce promoted the formation of (Mn0.58Fe0.42)2O3 and Al enhanced the surface acidity sites and active species dispersion.•Sm raised the fraction of Mn3+ and Ce3+ and suppressed SO2 poisoning by hindering electron transfer between M4+ and SO2. |
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ISSN: | 2213-3437 2213-3437 |
DOI: | 10.1016/j.jece.2022.107772 |