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Ammonia-Free Selective Catalytic Reduction of NO at Low Temperature on Melamine Impregnated MnOx–CeO2/Carbon Aerogels
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2021-09-05 , DOI: 10.1021/acs.iecr.1c03010
Xiaomin Cheng 1 , Xixi Xiao 1 , Yan Yin 1 , Jitong Wang 1, 2 , Wenming Qiao 1, 2 , Licheng Ling 1, 2
Affiliation  

Ammonia selective catalytic reduction (NH3-SCR), the most applied technology for abating emissions of NOx, frequently suffers from serious leakage of NH3 and high operating temperatures. In order to overcome these limitations, melamine impregnated MnOx–CeO2/carbon aerogels were synthesized by the incipient wetness impregnation method for low-temperature NH3-free SCR of NO. The combination of carbon aerogels with highly interconnected mesoporous structures and uniform dispersed MnOx–CeO2 can not only promote the chemisorption of nitrogen oxides but also increase the amounts of active metal sites and surface chemisorbed oxygen. Moreover, the impregnated melamine as reductant instead of NH3 is effective to eliminate NO, avoiding the secondary pollution derived from the escape of NH3. Therefore, the catalyst 400-12(Mn–Ce)/QS-15mel exhibits outstanding activity with 100% steady state NOx conversion for 7 h at 185 °C. Mechanism analysis indicates that melamine-SCR is accompanied by the variation of −NH2 and the generation of adsorbed HNCO, which could further participate in the reduction of NO without any byproducts. This work gives an in-depth understanding of the reactivity and mechanism of melamine-SCR and offers a novel route for the design of highly efficient catalysts.

中文翻译:

三聚氰胺浸渍的MnOx-CeO2/碳气凝胶在低温下无氨选择性催化还原NO

氨选择性催化还原(NH 3 -SCR)是应用最多的减少NO x排放的技术,但经常遭受NH 3泄漏严重和工作温度高的问题。为了克服这些限制,三聚氰胺浸渍的MnO x -CeO 2 /碳气凝胶通过初湿浸渍法合成,用于NO的低温无NH 3 SCR。具有高度互连的介孔结构和均匀分散的 MnO x –CeO 2的碳气凝胶的组合不仅可以促进氮氧化物的化学吸附,而且可以增加活性金属位点和表面化学吸附氧的数量。此外,浸渍三聚氰胺作为还原剂代替NH 3可有效去除NO,避免NH 3逸出造成的二次污染。因此,催化剂400-12(MN 6)/ QS-15mel展品,用100%的稳态NO优秀活性X在185转换为7小时℃。机理分析表明,三聚氰胺-SCR伴随着-NH 2的变化并产生吸附的HNCO,可进一步参与NO的还原,且无任何副产物。这项工作深入了解了三聚氰胺-SCR的反应性和机理,并为设计高效催化剂提供了一条新途径。
更新日期:2021-09-15
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