{"title":"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","authors":"Ze-rong HAO , Shuo FENG , Yu-ye XING , Bo-xiong SHEN","doi":"10.1016/S1872-5813(23)60358-5","DOIUrl":null,"url":null,"abstract":"<div><p>A series of Mn/CeO<sub>2</sub> 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 Fe<sub>5</sub>Mn/CeO<sub>2</sub> 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, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD and O<sub>2</sub>-TPD. XPS results showed that the increased content of Ce<sup>3+</sup> and Mn<sup>4+</sup> in the Fe<sub>5</sub>Mn/CeO<sub>2</sub> 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, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD and O<sub>2</sub>-TPD indicate that Fe<sub>5</sub>Mn/CeO<sub>2</sub> catalyst has great redox ability, stronger acidity and better oxygen migration ability. In addition, this paper explores the effects between selective catalytic reduction (NH<sub>3</sub>-SCR) and catalytic oxidation reaction of toluene over Fe<sub>5</sub>Mn/CeO<sub>2</sub> catalyst. NH<sub>3</sub> 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 NH<sub>3</sub>-SCR process in a certain temperature range. While NO promotes the formation of NO<sub>2</sub>, NO<sub>2</sub> effectively promotes the combination of toluene and active sites, which is conducive to the catalytic oxidation of toluene; The inhibition of toluene on the NH<sub>3</sub>-SCR process weakens with the increase of temperature. At 100 °C, the inhibition of toluene on the NH<sub>3</sub>-SCR process disappears. When the temperature exceeds 225 °C, toluene reacts with NO as a reducing agent and promotes the formation of NO<sub>2</sub>, thus promoting the NH<sub>3</sub>-SCR reaction.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"51 12","pages":"Pages 1866-1878"},"PeriodicalIF":0.0000,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Experimental study of Fe modified Mn/CeO2 catalyst for simultaneous removal of NO and toluene at low temperature\",\"authors\":\"Ze-rong HAO , Shuo FENG , Yu-ye XING , Bo-xiong SHEN\",\"doi\":\"10.1016/S1872-5813(23)60358-5\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A series of Mn/CeO<sub>2</sub> 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 Fe<sub>5</sub>Mn/CeO<sub>2</sub> 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, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD and O<sub>2</sub>-TPD. XPS results showed that the increased content of Ce<sup>3+</sup> and Mn<sup>4+</sup> in the Fe<sub>5</sub>Mn/CeO<sub>2</sub> 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, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD and O<sub>2</sub>-TPD indicate that Fe<sub>5</sub>Mn/CeO<sub>2</sub> catalyst has great redox ability, stronger acidity and better oxygen migration ability. In addition, this paper explores the effects between selective catalytic reduction (NH<sub>3</sub>-SCR) and catalytic oxidation reaction of toluene over Fe<sub>5</sub>Mn/CeO<sub>2</sub> catalyst. NH<sub>3</sub> 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 NH<sub>3</sub>-SCR process in a certain temperature range. While NO promotes the formation of NO<sub>2</sub>, NO<sub>2</sub> effectively promotes the combination of toluene and active sites, which is conducive to the catalytic oxidation of toluene; The inhibition of toluene on the NH<sub>3</sub>-SCR process weakens with the increase of temperature. At 100 °C, the inhibition of toluene on the NH<sub>3</sub>-SCR process disappears. When the temperature exceeds 225 °C, toluene reacts with NO as a reducing agent and promotes the formation of NO<sub>2</sub>, thus promoting the NH<sub>3</sub>-SCR reaction.</p></div>\",\"PeriodicalId\":15956,\"journal\":{\"name\":\"燃料化学学报\",\"volume\":\"51 12\",\"pages\":\"Pages 1866-1878\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2023-12-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"燃料化学学报\",\"FirstCategoryId\":\"1087\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872581323603585\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"Energy\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"燃料化学学报","FirstCategoryId":"1087","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872581323603585","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"Energy","Score":null,"Total":0}
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.
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.