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新型芦苇花状 SmMnO 催化剂的合成及其低温活性和抗 SO2 性能增强用于 NH3-SCR。

Novel synthesis of reed flower-like SmMnO catalyst with enhanced low-temperature activity and SO resistance for NH-SCR.

机构信息

School of Chemistry and Environment, Yunnan Minzu University, Kunming, 650505, China.

School of Chemistry and Environment, Yunnan Minzu University, Kunming, 650505, China; State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Kunming University of Science and Technology, Kunming, 650093, China.

出版信息

Environ Res. 2022 Dec;215(Pt 1):114231. doi: 10.1016/j.envres.2022.114231. Epub 2022 Sep 7.

Abstract

In this work, a novel co-precipitation coupled solvothermal procedure is proposed to prepare a SmMnO catalyst (SmMnOx-CP + ST) with a reed flower-like structure for the selective catalytic reduction of NO by NH (NH-SCR). Over 90% NO conversion and N selectivity was achieved at a low temperature range (25-200 °C), and 96% NO conversion was achieved in the presence of 100 ppm SO at 75 °C. While the NH-SCR of the SmMnO catalysts prepared by co-precipitation (SmMnO-CP) and solvothermal (SmMnO-ST) methods performed much poorer than the SmMnO-CP + ST catalyst. All catalysts were characterized by XRD, BET, SEM, XPS, H-TPR, NH-TPD, NO-TPD, and FT-IR. The results revealed that the superior performance of the SmMnO-CP + ST is due to the unique reed flower-like structure morphology, which endows the SmMnO-CP + ST with the largest surface area, the strongest synergistic reaction of Sm and Mn, abundant surface oxygen species and surface active sites, and significantly enhances the redox ability. Furthermore, the amorphous reed flower-like structure showed strong short-range ordered interaction between the active components and weaken the formation of sulfates species. In addition, the highest content of Mn and Mn+Mn greatly promotes the redox cycles of Sm↔Mn and Sm↔Mn, and suppresses the production of sulfate species in the presence of SO.

摘要

在这项工作中,提出了一种新颖的共沉淀耦合溶剂热法来制备具有芦苇花状结构的 SmMnO 催化剂(SmMnOx-CP + ST),用于 NH 选择性催化还原 NO(NH-SCR)。在较低的温度范围内(25-200°C)实现了超过 90%的 NO 转化率和 N 选择性,并且在 75°C 时存在 100ppm SO 的情况下实现了 96%的 NO 转化率。而通过共沉淀(SmMnO-CP)和溶剂热(SmMnO-ST)方法制备的 SmMnO 催化剂的 NH-SCR 性能远不如 SmMnO-CP + ST 催化剂。所有催化剂均通过 XRD、BET、SEM、XPS、H-TPR、NH-TPD、NO-TPD 和 FT-IR 进行了表征。结果表明,SmMnO-CP + ST 的优异性能归因于独特的芦苇花状结构形态,该形态赋予了 SmMnO-CP + ST 最大的表面积、Sm 和 Mn 的最强协同反应、丰富的表面氧物种和表面活性位,并显著增强了氧化还原能力。此外,无定形的芦苇花状结构表现出活性成分之间强烈的短程有序相互作用,从而削弱了硫酸盐物种的形成。此外,Mn 和 Mn+Mn 的含量最高促进了 Sm↔Mn 和 Sm↔Mn 的氧化还原循环,并抑制了 SO 存在下硫酸盐物种的生成。

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