K+诱导Mn-Ce固溶体增强酸性和活性氧协同促进NH3-SCR

陈曦; 王小燕; 李巧艳; 王梦雪; 梁美生

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中国环境科学 ›› 2024, Vol. 44 ›› Issue (11) : 6036-6046.

大气污染与控制

K⁺诱导Mn-Ce固溶体增强酸性和活性氧协同促进NH₃-SCR

陈曦^1,2, 王小燕¹, 李巧艳¹, 王梦雪¹, 梁美生¹

作者信息 +

The synergy between K⁺-induced enhanced acidity and active oxygen in Mn-Ce solid solution for promotion of NH₃-SCR

CHEN Xi^1,2, WANG Xao-yan¹, LI Qiao-yan¹, WANG Meng-xue¹, LIANG Mei-sheng¹

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摘要

In this work, K ions were successfully introduced into the lattice of as-prepared Mn-Ce solid solutions (MnCeO_x) 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 MnCeK_yO_x on NH₃-SCR. With the proportion of 1:5:5 for the amounts of K, Ce and Mn elements, the best performed catalyst MnCeK₁O_x 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 MnCeO_x and MnCeK₁O_x suggested that the reaction was more sensitive to the adsorption of NH₃ than NO. For MnCeO_x, NH₃ was primarily bound on Lewis then Brønsted acid sites, resulting in the rapid aggregation of both monodentate and bidentate nitrate. For MnCeK₁O_x, 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.

Abstract

导出引用

陈曦, 王小燕, 李巧艳, 王梦雪, 梁美生. K⁺诱导Mn-Ce固溶体增强酸性和活性氧协同促进NH₃-SCR[J]. 中国环境科学. 2024, 44(11): 6036-6046

CHEN Xi, WANG Xao-yan, LI Qiao-yan, WANG Meng-xue, LIANG Mei-sheng. The synergy between K⁺-induced enhanced acidity and active oxygen in Mn-Ce solid solution for promotion of NH₃-SCR[J]. China Environmental Science. 2024, 44(11): 6036-6046

中图分类号： X511

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