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SO对双功能NiMnO-CeO催化剂上同时去除NO和丙烷的影响机制

Mechanism of SO effect on the simultaneous removal of NO and propane over bifunctional NiMnO-CeO catalysts.

作者信息

Ma Shuang, Hou Yaqin, Yang Yatao, Li Yifan, Li Biao, Cui Yan, Chen Haijun, Huang Zhanggen

机构信息

State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, PR China; University of Chinese Academy of Sciences, Beijing 100049, PR China.

State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, PR China; University of Chinese Academy of Sciences, Beijing 100049, PR China.

出版信息

J Hazard Mater. 2024 Dec 5;480:136473. doi: 10.1016/j.jhazmat.2024.136473. Epub 2024 Nov 13.

Abstract

Nitrogen oxides (NO) and volatile organic compounds (VOCs) are the main pollutants in flue gas, and the synergistic removal of NO and VOCs in the presence of SO is still a challenge. In this work, the microstructure of NiMnO-CeO catalysts and the distribution of sulfur-containing substances were studied to reveal the inactivation mechanism of sulfur poisoning. NO conversion could reach more than 80 % at 100-250 °C, and CH conversion could achieve 90 % at 210 °C in the synergistic reaction on NiMnO-CeO catalyst, which has dual active sites with propane oxidation and SCR reactions carried out at Mn and Ni sites, respectively. In addition, the intrinsic effect of SO on propane oxidation and NO reduction were investigated by decoupling. For propane oxidation, mechanistic studies have shown that manganese sulfate generated by SO hindered further reactions by inhibiting the breaking of the CC bond. For denitration reaction, the generation of sulfate not only resulted in electron transfer from Ni to Mn thereby reducing reaction activity, but also blocked the L-H pathway by inhibiting NO adsorption. This work provides guidelines and strategies to mitigate SO poisoning in the simultaneous removal of NO and light alkane.

摘要

氮氧化物(NO)和挥发性有机化合物(VOCs)是烟气中的主要污染物,在SO存在下协同去除NO和VOCs仍然是一项挑战。在这项工作中,研究了NiMnO-CeO催化剂的微观结构和含硫物质的分布,以揭示硫中毒的失活机制。在NiMnO-CeO催化剂上的协同反应中,100-250°C时NO转化率可达80%以上,210°C时CH转化率可达90%,该催化剂具有双活性位点,丙烷氧化和SCR反应分别在Mn和Ni位点进行。此外,通过解耦研究了SO对丙烷氧化和NO还原的内在影响。对于丙烷氧化,机理研究表明,SO生成的硫酸锰通过抑制C-C键的断裂阻碍了进一步反应。对于脱硝反应,硫酸盐的生成不仅导致电子从Ni转移到Mn从而降低反应活性,还通过抑制NO吸附阻断了L-H途径。这项工作为在同时去除NO和轻质烷烃过程中减轻SO中毒提供了指导方针和策略。

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