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Insight into the activity and SO2 tolerance of hierarchically ordered MnFe1-δCoδOx ternary oxides for low-temperature selective catalytic reduction of NOx with NH3
Journal of Catalysis ( IF 7.3 ) Pub Date : 2021-01-06 , DOI: 10.1016/j.jcat.2020.12.036
Yonglong Li , Senyou Yang , Honggen Peng , Wenming Liu , Yangyang Mi , Zheng Wang , Changjin Tang , Daishe Wu , Taicheng An

Manganese (Mn)-based mixed oxides are considered the most efficient catalysts for low-temperature ammonia selective catalytic reduction of nitrogen oxides (NOx) (NH3-SCR of NOx). Water resistance and sulfur tolerance, especially the SO2 tolerance of Mn-based catalysts, are the main obstacles preventing their practical application. Therefore, in this study, a series of cobalt (Co)-doped MnFeOx ternary mixed oxides catalysts with a hierarchically ordered structure (Hierc-MnFe1-δCoδOx, δ = 0.2, 0.4 and 0.6) were developed and applied for NH3-SCR of NOx at low temperature. Compared with Hierc-MnFeOx, Hierc-MnFe1-δCoδOx catalyst exhibited enhanced low-temperature activity and a broadened temperature window (NOx conversion above 80% was between 90 and 343 °C over Hierc-MnFe0.6Co0.4Ox), as well as better H2O resistance and SO2 tolerance. The enhanced low-temperature activity was attributed to a larger amount of active oxygen species, a higher proportion of Mn4+, Fe3+ and Co3+ content, and the improvement of surface acidity, which can facilitate the adsorption and activation of NO and NH3. Additionally, the Hierc-MnFe0.6Co0.4Ox catalyst exhibited superior soot tolerance due to its special hierarchically ordered architecture. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) revealed that the Co-modified Hierc-MnFe1-δCoδOx ternary oxide catalyst could efficiently protect nitrate species on Hierc-MnFe0.6Co0.4Ox from the poisoning effect of SO2, thereby boosting its SO2 tolerance. This study provides a good candidate for low-temperature deNOx application with enhanced SO2 and soot tolerance.



中文翻译:

洞察活性和SO 2公差的分级排序的锰铁1-δδ ø X三元氧化物为NO的低温选择性催化还原X与NH 3

锰(Mn)基混合氧化物被认为是低温氨选择性催化还原氮氧化物(NO的最有效的催化剂X)(NH 3 -SCR NO的X)。耐水性和耐硫性,特别是Mn基催化剂的SO 2耐性是阻碍其实际应用的主要障碍。因此,在该研究中,一系列钴(Co) -掺杂的MnFeO X三元具有层次有序结构的混合氧化物的催化剂(Hierc-锰铁1-δδ ø X,δ= 0.2,0.4和0.6)进行了开发和应用对于NH 3 -SCR的NO x在低温下。与Hierc-MnFeO相比X,Hierc-锰铁1-δδ ø X催化剂表现出增强的低温活性和加宽的温度窗口(NO X转化率在80%以上为90和343℃之间在Hierc-锰铁0.60.4 O x),以及更好的H 2 O耐受性和SO 2耐受性。增强的低温活性归因于大量的活性氧,较高比例的Mn 4+,Fe 3+和Co 3+含量和表面酸性的改善,这可以促进NO和NH 3的吸附和活化。另外,Hierc-MnFe 0.6 Co 0.4 O x催化剂由于其特殊的分级有序结构而显示出优异的烟尘耐受性。原位漫反射红外线傅里叶变换光谱法(DRIFTS)分析表明共改性Hierc-锰铁1-δδ ø X三元氧化物催化剂可以在Hierc-锰铁有效地保护硝酸盐物种0.60.4 ø X从SO的中毒效果2,从而提高其SO 2公差。这项研究为低温x的应用提供了一个很好的候选者,它具有增强的SO 2和烟灰耐受性。

更新日期:2021-02-01
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