铁改性 Mn/CeO2 催化剂在低温下同时去除 NO 和甲苯的实验研究

Q3 Energy 燃料化学学报 Pub Date : 2023-12-01 DOI:10.1016/S1872-5813(23)60358-5
Ze-rong HAO , Shuo FENG , Yu-ye XING , Bo-xiong SHEN
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引用次数: 0

摘要

采用浸渍法制备了一系列不同铁含量改性的 Mn/CeO2 催化剂,并对其同时脱硝和脱甲苯的低温性能进行了测试。结果发现,Fe5Mn/CeO2 催化剂的催化性能最好,在 175 ℃ 时甲苯的转化率达到 90%,在 95-300 ℃ 时氮氧化物的转化率达到 90%。催化剂的物理和化学特性由 BET、SEM、XRD、XPS、H2-TPR、NH3-TPD 和 O2-TPD 表征。XPS 结果表明,Fe5Mn/CeO2 催化剂中 Ce3+ 和 Mn4+ 含量的增加促进了氧空位和不饱和化学键的形成,提供了更多的活性位点,从而有利于在低温下高效去除 NO 和甲苯。与其他催化剂相比,H2-TPR、NH3-TPD 和 O2-TPD 表明 Fe5Mn/CeO2 催化剂具有很强的氧化还原能力,酸性更强,氧迁移能力更强。此外,本文还探讨了 Fe5Mn/CeO2 催化剂对甲苯的选择性催化还原(NH3-SCR)和催化氧化反应的影响。NH3 优先与催化剂上的活性位点反应,抑制甲苯氧化过程,而 NO 则促进甲苯脱除过程。甲苯可在一定温度范围内促进 NH3-SCR 过程。NO 促进 NO2 的形成,而 NO2 则有效促进甲苯与活性位点的结合,有利于甲苯的催化氧化;甲苯对 NH3-SCR 过程的抑制作用随着温度的升高而减弱。在 100 ℃ 时,甲苯对 NH3-SCR 过程的抑制作用消失。当温度超过 225 ℃ 时,甲苯作为还原剂与 NO 发生反应,促进 NO2 的生成,从而促进 NH3-SCR 反应。
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Experimental study of Fe modified Mn/CeO2 catalyst for simultaneous removal of NO and toluene at low temperature

A series of Mn/CeO2 catalysts modified with different Fe contents were prepared by impregnation method and tested for their low-temperature performance for simultaneous de-nitrification and toluene removal. It was found that the Fe5Mn/CeO2 catalyst showed the best catalytic performance and the conversion efficiency of toluene reached 90% at 175 °C and NO conversion reached 90% at 95−300 °C. The physical and chemical properties of the catalysts were characterized by BET, SEM, XRD, XPS, H2-TPR, NH3-TPD and O2-TPD. XPS results showed that the increased content of Ce3+ and Mn4+ in the Fe5Mn/CeO2 catalyst promoted the formation of oxygen vacancies and unsaturated chemical bonds, providing more active sites, thus facilitating the efficient removal of NO and toluene at low temperatures. Compared with other catalysts, H2-TPR, NH3-TPD and O2-TPD indicate that Fe5Mn/CeO2 catalyst has great redox ability, stronger acidity and better oxygen migration ability. In addition, this paper explores the effects between selective catalytic reduction (NH3-SCR) and catalytic oxidation reaction of toluene over Fe5Mn/CeO2 catalyst. NH3 preferentially reacts with the active site on the catalyst to inhibit the toluene oxidation process, while NO promotes the toluene removal process. Toluene can promote the NH3-SCR process in a certain temperature range. While NO promotes the formation of NO2, NO2 effectively promotes the combination of toluene and active sites, which is conducive to the catalytic oxidation of toluene; The inhibition of toluene on the NH3-SCR process weakens with the increase of temperature. At 100 °C, the inhibition of toluene on the NH3-SCR process disappears. When the temperature exceeds 225 °C, toluene reacts with NO as a reducing agent and promotes the formation of NO2, thus promoting the NH3-SCR reaction.

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来源期刊
燃料化学学报
燃料化学学报 Chemical Engineering-Chemical Engineering (all)
CiteScore
2.80
自引率
0.00%
发文量
5825
期刊介绍: Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.
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