Yupeng WANG , Youkang MA , Yonggang ZHAO , Peng CAO
{"title":"Study on the improvement of ultra-low temperature performance and adsorption mechanism of Mn and Ce based denitrification catalysts by “NO2 SCR”","authors":"Yupeng WANG , Youkang MA , Yonggang ZHAO , Peng CAO","doi":"10.1016/S1872-5813(24)60487-1","DOIUrl":null,"url":null,"abstract":"<div><div>The catalysts supported by Mn<sub>7</sub>Fe<sub>4</sub>Ce<sub>9</sub>O<sub><em>x</em></sub>/AlO<sub><em>x</em></sub> and Mn<sub>3</sub>Fe<sub>1</sub>Ce<sub>6</sub>O<sub><em>x</em></sub>/AlO<sub><em>x</em></sub> prepared by co-precipitation method were first evaluated by standard SCR mechanism reaction under 7777 h<sup>–1</sup> intake condition. The catalytic activity of the two catalysts was only about 10% at 60 °C. Then, the concentration ratio of NO<sub>2</sub>/NO<sub><em>x</em></sub> in intake air was increased under the same conditions, and the concentration ratio of NO<sub>2</sub>/NO<sub><em>x</em></sub> in intake air was 0, 14.3%, 28.6%, 42.8%, 57%, 71.4%, 85.7% and 100%. The results show that the denitrification efficiency of Mn<sub>3</sub>Fe<sub>1</sub>Ce<sub>6</sub>O<sub><em>x</em></sub>/AlO<sub><em>x</em></sub> catalyst can be 64% at 60 °C, which is about 58% higher than that of the first evaluation. Experimental and theoretical calculations show that Mn<sub>3</sub>Fe<sub>1</sub>Ce<sub>6</sub>O<sub><em>x</em></sub>/AlO<sub><em>x</em></sub> catalyst has larger specific surface area and stronger adsorption and activation of NO<sub>2</sub>, which improves the efficiency of NO<sub>2</sub> fast SCR mechanism reaction. At the same time, the <em>in-situ</em> infrared test found that the adsorption mode of Mn<sub>3</sub>Fe<sub>1</sub>Ce<sub>6</sub>O<sub><em>x</em></sub>/AlO<sub><em>x</em></sub> catalyst changed significantly when the concentration ratio of NO<sub>2</sub>/NO<sub><em>x</em></sub> increased, and the E-R and L-H mechanism mainly adsorbed by NH<sub>3</sub> changed to the E-R and L-H mechanism mainly adsorbed by NO<sub>2</sub>. The change of adsorption mechanism may be the key factor to improve the performance of catalyst at ultra-low temperature. This work provides a promising strategy for exploring efficient and economical denitrification of NH<sub>3</sub>-SCR, as well as experience for ultra-low temperature flue gas treatment and guidance for new flue gas treatment processes.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 1","pages":"Pages 138-151"},"PeriodicalIF":0.0000,"publicationDate":"2025-01-01","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/S1872581324604871","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"Energy","Score":null,"Total":0}
引用次数: 0
Abstract
The catalysts supported by Mn7Fe4Ce9Ox/AlOx and Mn3Fe1Ce6Ox/AlOx prepared by co-precipitation method were first evaluated by standard SCR mechanism reaction under 7777 h–1 intake condition. The catalytic activity of the two catalysts was only about 10% at 60 °C. Then, the concentration ratio of NO2/NOx in intake air was increased under the same conditions, and the concentration ratio of NO2/NOx in intake air was 0, 14.3%, 28.6%, 42.8%, 57%, 71.4%, 85.7% and 100%. The results show that the denitrification efficiency of Mn3Fe1Ce6Ox/AlOx catalyst can be 64% at 60 °C, which is about 58% higher than that of the first evaluation. Experimental and theoretical calculations show that Mn3Fe1Ce6Ox/AlOx catalyst has larger specific surface area and stronger adsorption and activation of NO2, which improves the efficiency of NO2 fast SCR mechanism reaction. At the same time, the in-situ infrared test found that the adsorption mode of Mn3Fe1Ce6Ox/AlOx catalyst changed significantly when the concentration ratio of NO2/NOx increased, and the E-R and L-H mechanism mainly adsorbed by NH3 changed to the E-R and L-H mechanism mainly adsorbed by NO2. The change of adsorption mechanism may be the key factor to improve the performance of catalyst at ultra-low temperature. This work provides a promising strategy for exploring efficient and economical denitrification of NH3-SCR, as well as experience for ultra-low temperature flue gas treatment and guidance for new flue gas treatment processes.
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.