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The synergy between K+-induced enhanced acidity and active oxygen in Mn-Ce solid solution for promotion of NH3-SCR |
CHEN Xi1,2, WANG Xao-yan1, LI Qiao-yan1, WANG Meng-xue1, LIANG Mei-sheng1 |
1. Shanxi Key Laboratory of Compound Air Pollutions Identification and Control, College of Environmental Science and Engineering, Taiyuan University of Technology, Jinzhong 030600, China; 2. Shanxi Academy of Eco-Environmental Planning and Technology, Taiyuan 030009, China |
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Abstract In this work, K ions were successfully introduced into the lattice of as-prepared Mn-Ce solid solutions (MnCeOx) by a hydrothermal method, and that was applied in NH3-SCR. The Mn-O bonding was deeply weakened, leading to a better reducibility and oxygen desorption capacity of the K-contained catalysts according to H2-TPR and O2-TPD. Furthermore, the introduction of K ions could facilitate the adsorptive capacity of Brønsted acid sites for NH3 due to the enhanced electron transfer between Mn/Ce elements according to the characterizations of XPS, NH3-TPD and in situ DRIFT. Then, the synergy among the acidity and adsorbed active oxygen could promote the activities of catalyst MnCeKyOx on NH3-SCR. With the proportion of 1:5:5 for the amounts of K, Ce and Mn elements, the best performed catalyst MnCeK1Ox could achieve 94.6% conversion of NO at a lower temperature of 120℃. The broader temperature ranging from 40~260℃ is beneficial for the conversion of NO at many conditions. Finally, in situ DRIFTs of NH3 and NO adsorption on MnCeOx and MnCeK1Ox suggested that the reaction was more sensitive to the adsorption of NH3 than NO. For MnCeOx, NH3 was primarily bound on Lewis then Brønsted acid sites, resulting in the rapid aggregation of both monodentate and bidentate nitrate. For MnCeK1Ox, the simultaneous adsorption of NH3 on Lewis and Brønsted acid sites led to less accumulation of intermediates like bidentate nitrate. The results indicated that the introduction of K ions could efficiently improve the activity of Mn-Ce solid solution in NH3-SCR reaction.
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Received: 25 March 2024
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