{"title":"通过控制 MnaNbTi2Ox(a = 0.6-0.9)催化剂上的锰/铌比来调节 NH3 氧化和抑制硫酸盐沉积,从而提高 NH3-SCR 脱硝性能","authors":"Yushi Li, Xuesong Leng, Zhiping Zhang, Xiaoyu Niu, Yujun Zhu","doi":"10.1016/j.jhazmat.2024.136568","DOIUrl":null,"url":null,"abstract":"The Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> (a = 0.6-0.9) catalysts for NH<sub>3</sub> selective catalytic reduction denitration were prepared using the co-precipitation method. Among them, Mn<sub>0.7</sub>NbTi<sub>2</sub>O<sub>x</sub> exhibits well low-temperature catalytic performance, wide activity temperature range (180-480 ℃), and worthy resistance to SO<sub>2</sub> even with H<sub>2</sub>O. XRD was used to investigate the structure of Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub>, in which Mn and Nb oxides highly dispersed in the Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> catalysts and Nb can dope into the crystal lattice of TiO<sub>2</sub>. XRF and XPS results show Nb can affect the transfer of electrons to Mn<sup>4+</sup>, and changing the Mn/Nb ratio can regulate the Mn<sup>4+</sup> content on the Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> catalysts. H<sub>2</sub>-TPR, NH<sub>3</sub> and NO oxidation results verify that Nb inhibits the oxidation capacity of Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub>, and altering the Mn/Nb ratio can get appropriate oxidation property, which facilitates low-temperature NH<sub>3</sub> activation and limit non-selective oxidation for NH<sub>3</sub>. <em>In-situ</em> DRIFTS results show Nb-OH bonds can provide new Brønsted acid sites, and both Lewis and Brønsted acid sites are active. Furthermore, Nb addition prevents sulphate deposition on the catalyst. The effect of Mn/Nb on catalytic performance, N<sub>2</sub>O formation and inhibition, SO<sub>2</sub> poisoning, SO<sub>2</sub> effect on NH<sub>3</sub>-SCR, and the enhancement of SO<sub>2</sub> tolerance are also analyzed.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"1 1","pages":""},"PeriodicalIF":12.2000,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Modulating NH3 oxidation and inhibiting sulfate deposition to improve NH3-SCR denitration performance by controlling Mn/Nb ratio over MnaNbTi2Ox (a = 0.6-0.9) catalysts\",\"authors\":\"Yushi Li, Xuesong Leng, Zhiping Zhang, Xiaoyu Niu, Yujun Zhu\",\"doi\":\"10.1016/j.jhazmat.2024.136568\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> (a = 0.6-0.9) catalysts for NH<sub>3</sub> selective catalytic reduction denitration were prepared using the co-precipitation method. Among them, Mn<sub>0.7</sub>NbTi<sub>2</sub>O<sub>x</sub> exhibits well low-temperature catalytic performance, wide activity temperature range (180-480 ℃), and worthy resistance to SO<sub>2</sub> even with H<sub>2</sub>O. XRD was used to investigate the structure of Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub>, in which Mn and Nb oxides highly dispersed in the Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> catalysts and Nb can dope into the crystal lattice of TiO<sub>2</sub>. XRF and XPS results show Nb can affect the transfer of electrons to Mn<sup>4+</sup>, and changing the Mn/Nb ratio can regulate the Mn<sup>4+</sup> content on the Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> catalysts. H<sub>2</sub>-TPR, NH<sub>3</sub> and NO oxidation results verify that Nb inhibits the oxidation capacity of Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub>, and altering the Mn/Nb ratio can get appropriate oxidation property, which facilitates low-temperature NH<sub>3</sub> activation and limit non-selective oxidation for NH<sub>3</sub>. <em>In-situ</em> DRIFTS results show Nb-OH bonds can provide new Brønsted acid sites, and both Lewis and Brønsted acid sites are active. Furthermore, Nb addition prevents sulphate deposition on the catalyst. The effect of Mn/Nb on catalytic performance, N<sub>2</sub>O formation and inhibition, SO<sub>2</sub> poisoning, SO<sub>2</sub> effect on NH<sub>3</sub>-SCR, and the enhancement of SO<sub>2</sub> tolerance are also analyzed.\",\"PeriodicalId\":361,\"journal\":{\"name\":\"Journal of Hazardous Materials\",\"volume\":\"1 1\",\"pages\":\"\"},\"PeriodicalIF\":12.2000,\"publicationDate\":\"2024-11-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Hazardous Materials\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jhazmat.2024.136568\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Hazardous Materials","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1016/j.jhazmat.2024.136568","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Modulating NH3 oxidation and inhibiting sulfate deposition to improve NH3-SCR denitration performance by controlling Mn/Nb ratio over MnaNbTi2Ox (a = 0.6-0.9) catalysts
The MnaNbTi2Ox (a = 0.6-0.9) catalysts for NH3 selective catalytic reduction denitration were prepared using the co-precipitation method. Among them, Mn0.7NbTi2Ox exhibits well low-temperature catalytic performance, wide activity temperature range (180-480 ℃), and worthy resistance to SO2 even with H2O. XRD was used to investigate the structure of MnaNbTi2Ox, in which Mn and Nb oxides highly dispersed in the MnaNbTi2Ox catalysts and Nb can dope into the crystal lattice of TiO2. XRF and XPS results show Nb can affect the transfer of electrons to Mn4+, and changing the Mn/Nb ratio can regulate the Mn4+ content on the MnaNbTi2Ox catalysts. H2-TPR, NH3 and NO oxidation results verify that Nb inhibits the oxidation capacity of MnaNbTi2Ox, and altering the Mn/Nb ratio can get appropriate oxidation property, which facilitates low-temperature NH3 activation and limit non-selective oxidation for NH3. In-situ DRIFTS results show Nb-OH bonds can provide new Brønsted acid sites, and both Lewis and Brønsted acid sites are active. Furthermore, Nb addition prevents sulphate deposition on the catalyst. The effect of Mn/Nb on catalytic performance, N2O formation and inhibition, SO2 poisoning, SO2 effect on NH3-SCR, and the enhancement of SO2 tolerance are also analyzed.
期刊介绍:
The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.