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Sm/Zr共掺杂
CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Insights into the Sm/Zr co-doping effects on N2 selectivity and SO2 resistance of a MnOx-TiO2 catalyst for the NH3-SCR reaction

Chuanzhi Sun,Hao Liu,Wei Chen,Dezhan Chen,Shuohan Yu,Annai Liu,Lin Dong,Shuai Feng

A series of Sm- and/or Zr-doped MnO x -TiO 2 catalysts were prepared, and the catalysts exhibited better N 2 selectivity and SO 2 resistance than the undoped MnO x -TiO 2 catalyst for the selective catalytic reduction of NO by NH 3 (NH 3 -SCR). The reasons for the good N 2 selectivity and SO 2 resistance of the catalysts were proposed. X-ray photoelectron spectroscopy (XPS) combined with density functional theory (DFT) calculations suggested that electron transfer between the manganese and samarium species by Mn 4+  + Sm 2+  ↔ Mn 3+  + Sm 3+ redox cycles occurred in the Sm-containing catalysts. Furthermore, electron transfer from Sm 2+ to Mn 4+ suppressed electron transfer from NH 3 to Mn 4+ , inhibiting the formation of NH 2 or NH. Thus, the pathway for NH generation was removed, and the reaction of 2NH + 4NO → 3N 2 O + H 2 O was prevented. Consequently, the N 2 selectivity of the NH 3 -SCR reaction was enhanced. In situ diffused reflectance infrared Fourier transform spectroscopy ( in situ DRIFTS) combined with thermogravimetry, differential scanning calorimetry and mass spectrometry (TG-DSC-MS) results revealed that the deposition rate of sulfate species decreases after Sm doping, which was also attributed to the suppressed electron transfer from SO 2 to Mn 4+ , i.e., the oxidation of SO 2 to SO 3 . Thus, the catalysts exhibited better SO 2 resistance.

CAS / MDL: 13759-83-6
研究领域: 催化化学 · 环境科学
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