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Shengyang Zhang, Bolin Zhang, Boyu Wu, Bo Liu, and Shengen Zhang, Effect of samarium on the N2 selectivity of SmxMn0.3−xTi catalysts during selective catalytic reduction of NOx with NH3, Int. J. Miner. Metall. Mater., 30(2023), No. 4, pp.642-652. https://dx.doi.org/10.1007/s12613-021-2348-5
Shengyang Zhang, Bolin Zhang, Boyu Wu, Bo Liu, and Shengen Zhang, Effect of samarium on the N2 selectivity of SmxMn0.3−xTi catalysts during selective catalytic reduction of NOx with NH3, Int. J. Miner. Metall. Mater., 30(2023), No. 4, pp.642-652. https://dx.doi.org/10.1007/s12613-021-2348-5
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钐对SmxMn0.3−xTi催化剂NH3选择性催化还原NOx过程中N2选择性的影响

摘要: 本文研究了Sm对Mn基催化剂NH3选择性催化还原NO的改善作用。采用共沉淀法制备了一系列SmxMn0.3−xTi催化剂(x = 0, 0.1, 0.15, 0.2和0.3)。活性测试表明,Sm0.15Mn0.15Ti催化剂在180‒300°C条件下,NO转化率达100%,N2选择性达87%以上。表征结果表明,Mn基催化剂中添加Sm,抑制了TiO2和Mn2O3相的结晶,提高了比表面积和酸性,其中Sm改性催化剂的比表面积从152.2增加至241.7 m2·g−1。这些作用有利于提高催化活性。X射线光电子能谱(XPS)结果表明,Sm0.15Mn0.15Ti的Sm3+/Sm和Oβ/O的相对原子比分别为76.77at%和44.11at%,添加Sm增加了表面吸附氧(Oβ),降低了Mn4+的表面浓度;程序升温还原H2(H2-TPR)结果表明,Sm0.15Mn0.15Ti催化剂还原温度提高,H2消耗量降低至0.3 mmol⋅g−1。Sm的引入降低了催化剂Mn4+表面浓度,使得该催化剂氧化还原性能降低,进一步抑制NH3氧化和非选择性催化还原反应生成N2O,从而提高了催化剂的N2选择性。原位漫反射红外傅立叶变换光谱(DRIFTs)表明,Sm0.15Mn0.15Ti催化剂的NH3-SCR反应主要遵循Eley‒Rideal机制。Sm掺杂增加了Sm0.15Mn0.15Ti催化剂的表面吸附氧(Oβ),降低了氧化还原性能,提高了Sm0.15Mn0.15Ti催化剂的NO转化率和N2选择性。

 

Effect of samarium on the N2 selectivity of SmxMn0.3−xTi catalysts during selective catalytic reduction of NOx with NH3

Abstract: This work aims to study the improvement effect of Sm on Mn-based catalysts for selective catalytic reduction (SCR) of NO with NH3. A series of SmxMn0.3−xTi catalysts (x = 0, 0.1, 0.15, 0.2, and 0.3) were prepared by co-precipitation. Activity tests indicated that the Sm0.15Mn0.15Ti catalyst showed superior performances, with a NO conversion of 100% and N2 selectivity above 87% at 180–300°C. The characterizations showed that Sm doping suppressed the crystallization of TiO2 and Mn2O3 phases and increased the specific surface area and acidity. In particular, the surface area increased from 152.2 m2·g−1 for Mn0.3Ti to 241.7 m2·g−1 for Sm0.15Mn0.15Ti. These effects contributed to the high catalytic activity. The X-ray photoelectron spectroscopy (XPS) results indicated that the relative atomic ratios of Sm3+/Sm and Oβ/O of Sm0.15Mn0.15Ti were 76.77at% and 44.11at%, respectively. The presence of Sm contributed to an increase in surface-absorbed oxygen (Oβ) and a decrease in Mn4+ surface concentration, which improved the catalytic activity. In the results of hydrogen temperature-programmed reduction (H2-TPR), the presence of Sm induced a higher reduction temperature and lower H2 consumption (0.3 mmol·g−1) for the Sm0.15Mn0.15Ti catalyst compared to the Mn0.3Ti catalyst. The decrease in Mn4+ weakened the redox property of the catalysts and increased the N2 selectivity by suppressing N2O formation from NH3 oxidation and the nonselective catalytic reduction reaction. The in situ diffuse reflectance infrared Fourier transform spectra (DRIFTs) revealed that NH3-SCR of NO over the Sm0.15Mn0.15Ti catalyst mainly followed the Eley–Rideal mechanism. Sm doping increased surface-absorbed oxygen and weakened the redox property to improve the NO conversion and N2 selectivity of the Sm0.15Mn0.15Ti catalyst.

 

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