Miao Yu, Shuai Ji, Zhifang Li, Kun Song, Yueyu Li, Jian Yang, Changlong Yang
{"title":"Mn-Co共掺杂高活性TNU-9脱硝催化剂的合成与表征","authors":"Miao Yu, Shuai Ji, Zhifang Li, Kun Song, Yueyu Li, Jian Yang, Changlong Yang","doi":"10.1007/s12039-022-02059-9","DOIUrl":null,"url":null,"abstract":"<div><p>A simple ion-exchange method is used to prepare Mn and Co-supported TNU-9 denitration catalyst for NH<sub>3</sub>-SCR. The denitration activity and H<sub>2</sub>O/SO<sub>2</sub> resistance performance of the catalyst are systematically studied. The denitration activity test exhibits that the NO<sub>x</sub> removal rate of Mn-Co/TNU-9 is higher than that of Mn/TNU-9 and Co/TNU-9, the NO<sub>x</sub> removal rate is greater than 90% and the N<sub>2</sub> selectivity is greater than 99% in the range of 150 ~ 450 °C. It is because the redox cycle of Mn<sup>4+</sup> + Co<sup>2+</sup> ↔ Mn<sup>3+</sup> + Co<sup>3+</sup> improves the redox performance of the catalyst, which is conducive to the conduction of electrons, and then accelerates the oxidation of NO to NO<sub>2</sub> to produce a \"fast SCR\" reaction, and finally optimizes the overall SCR performance. Furthermore, the change is not significant for the catalytic activity over Mn-Co/TNU-9 in the presence of water. However, the sulfur resistance is poor at low temperatures due to the presence of ammonium bisulfate. It also has excellent catalytic stability. Therefore, supported TNU-9 catalysts will have a good development prospect in denitrification.</p><h3>Graphical abstract</h3><p>Mn-Co co-doped TNU-9 catalyst was successfully synthesized by simple ion exchange method and applied in the NH<sub>3</sub>-SCR. The results show that Mn-Co/TNU-9 catalyst has an excellent wide activity window in a wide temperature range of 150-450°C (NO<sub>x</sub> conversion over 90%), which is because Mn+Co<sup>2+</sup>↔Mn+Co improves the redox performance and facilitates the electron transfer, which further accelerates the oxidation of NO into NO<sub>2</sub> that could result in the “Fast SCR” reaction. The synergistic effect between Mn and Co bimetallic can also improve activity. Moreover, Mn-Co/TNU-9 has very good catalytic stability.\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"134 2","pages":""},"PeriodicalIF":1.7000,"publicationDate":"2022-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"2","resultStr":"{\"title\":\"Synthesis and characterization of Mn-Co co-doped TNU-9 denitration catalyst with high activity\",\"authors\":\"Miao Yu, Shuai Ji, Zhifang Li, Kun Song, Yueyu Li, Jian Yang, Changlong Yang\",\"doi\":\"10.1007/s12039-022-02059-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A simple ion-exchange method is used to prepare Mn and Co-supported TNU-9 denitration catalyst for NH<sub>3</sub>-SCR. The denitration activity and H<sub>2</sub>O/SO<sub>2</sub> resistance performance of the catalyst are systematically studied. The denitration activity test exhibits that the NO<sub>x</sub> removal rate of Mn-Co/TNU-9 is higher than that of Mn/TNU-9 and Co/TNU-9, the NO<sub>x</sub> removal rate is greater than 90% and the N<sub>2</sub> selectivity is greater than 99% in the range of 150 ~ 450 °C. It is because the redox cycle of Mn<sup>4+</sup> + Co<sup>2+</sup> ↔ Mn<sup>3+</sup> + Co<sup>3+</sup> improves the redox performance of the catalyst, which is conducive to the conduction of electrons, and then accelerates the oxidation of NO to NO<sub>2</sub> to produce a \\\"fast SCR\\\" reaction, and finally optimizes the overall SCR performance. Furthermore, the change is not significant for the catalytic activity over Mn-Co/TNU-9 in the presence of water. However, the sulfur resistance is poor at low temperatures due to the presence of ammonium bisulfate. It also has excellent catalytic stability. Therefore, supported TNU-9 catalysts will have a good development prospect in denitrification.</p><h3>Graphical abstract</h3><p>Mn-Co co-doped TNU-9 catalyst was successfully synthesized by simple ion exchange method and applied in the NH<sub>3</sub>-SCR. The results show that Mn-Co/TNU-9 catalyst has an excellent wide activity window in a wide temperature range of 150-450°C (NO<sub>x</sub> conversion over 90%), which is because Mn+Co<sup>2+</sup>↔Mn+Co improves the redox performance and facilitates the electron transfer, which further accelerates the oxidation of NO into NO<sub>2</sub> that could result in the “Fast SCR” reaction. The synergistic effect between Mn and Co bimetallic can also improve activity. Moreover, Mn-Co/TNU-9 has very good catalytic stability.\\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":50242,\"journal\":{\"name\":\"Journal of Chemical Sciences\",\"volume\":\"134 2\",\"pages\":\"\"},\"PeriodicalIF\":1.7000,\"publicationDate\":\"2022-05-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"2\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Chemical Sciences\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s12039-022-02059-9\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"Chemistry\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Sciences","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s12039-022-02059-9","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"Chemistry","Score":null,"Total":0}
Synthesis and characterization of Mn-Co co-doped TNU-9 denitration catalyst with high activity
A simple ion-exchange method is used to prepare Mn and Co-supported TNU-9 denitration catalyst for NH3-SCR. The denitration activity and H2O/SO2 resistance performance of the catalyst are systematically studied. The denitration activity test exhibits that the NOx removal rate of Mn-Co/TNU-9 is higher than that of Mn/TNU-9 and Co/TNU-9, the NOx removal rate is greater than 90% and the N2 selectivity is greater than 99% in the range of 150 ~ 450 °C. It is because the redox cycle of Mn4+ + Co2+ ↔ Mn3+ + Co3+ improves the redox performance of the catalyst, which is conducive to the conduction of electrons, and then accelerates the oxidation of NO to NO2 to produce a "fast SCR" reaction, and finally optimizes the overall SCR performance. Furthermore, the change is not significant for the catalytic activity over Mn-Co/TNU-9 in the presence of water. However, the sulfur resistance is poor at low temperatures due to the presence of ammonium bisulfate. It also has excellent catalytic stability. Therefore, supported TNU-9 catalysts will have a good development prospect in denitrification.
Graphical abstract
Mn-Co co-doped TNU-9 catalyst was successfully synthesized by simple ion exchange method and applied in the NH3-SCR. The results show that Mn-Co/TNU-9 catalyst has an excellent wide activity window in a wide temperature range of 150-450°C (NOx conversion over 90%), which is because Mn+Co2+↔Mn+Co improves the redox performance and facilitates the electron transfer, which further accelerates the oxidation of NO into NO2 that could result in the “Fast SCR” reaction. The synergistic effect between Mn and Co bimetallic can also improve activity. Moreover, Mn-Co/TNU-9 has very good catalytic stability.
期刊介绍:
Journal of Chemical Sciences is a monthly journal published by the Indian Academy of Sciences. It formed part of the original Proceedings of the Indian Academy of Sciences – Part A, started by the Nobel Laureate Prof C V Raman in 1934, that was split in 1978 into three separate journals. It was renamed as Journal of Chemical Sciences in 2004. The journal publishes original research articles and rapid communications, covering all areas of chemical sciences. A significant feature of the journal is its special issues, brought out from time to time, devoted to conference symposia/proceedings in frontier areas of the subject, held not only in India but also in other countries.