{"title":"Ce和Nb共掺杂提高MnOx催化剂的低温脱硝性能","authors":"Yanping Yang, Shengchen Li, Shunli Shi, Jie Hu, Zexi Xuchen, Shunmin Ding, Dan zhao, Shengjun Deng, Weiming Xiao, Shuhua Wang, Chao Chen","doi":"10.1016/j.seppur.2025.131768","DOIUrl":null,"url":null,"abstract":"Manganese oxide (MnO<sub>x</sub>) catalysts are promising for low-temperature NH<sub>3</sub>-Selective Catalytic Reduction (NH<sub>3</sub>-SCR) with their superior catalytic performance. However, the presence of alkali metals in flue gases, particularly potassium (K), leads to catalyst deactivation and limits their industrial application. This study investigates the synergistic effects of Ce and Nb doping on the K resistance and low-temperature NH<sub>3</sub>-SCR activity of MnO<sub>x</sub>. The surface acidity and redox properties of MnO<sub>x</sub> were modulated by Ce and Nb modification. In addition, the phase structure, surface state and active sites of the catalysts were characterized before and after K poisoning. The results indicated that Nb<sub>0.05</sub>Ce<sub>0.05</sub>MnO<sub>x</sub> exhibited exceptional low-temperature performance, achieving over 90 % NO conversion at 125-250°C, along with significant resistance to K poisoning·NH<sub>3</sub>-TPD and <em>in-situ</em> experiments revealed that the loss of acid sites is the primary cause of K poisoning. The mechanism follows the L-H mechanism with L-acid sites as the main active sites on the catalyst surface and bridging nitrate as the key intermediate state. This research provides valuable insights into enhancing the industrial applicability of MnO<sub>x-</sub>based catalysts for low-temperature denitrification.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.1000,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing the K-resistance of MnOx catalysts via Ce and Nb co-doping for low-temperature NOx elimination\",\"authors\":\"Yanping Yang, Shengchen Li, Shunli Shi, Jie Hu, Zexi Xuchen, Shunmin Ding, Dan zhao, Shengjun Deng, Weiming Xiao, Shuhua Wang, Chao Chen\",\"doi\":\"10.1016/j.seppur.2025.131768\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Manganese oxide (MnO<sub>x</sub>) catalysts are promising for low-temperature NH<sub>3</sub>-Selective Catalytic Reduction (NH<sub>3</sub>-SCR) with their superior catalytic performance. However, the presence of alkali metals in flue gases, particularly potassium (K), leads to catalyst deactivation and limits their industrial application. This study investigates the synergistic effects of Ce and Nb doping on the K resistance and low-temperature NH<sub>3</sub>-SCR activity of MnO<sub>x</sub>. The surface acidity and redox properties of MnO<sub>x</sub> were modulated by Ce and Nb modification. In addition, the phase structure, surface state and active sites of the catalysts were characterized before and after K poisoning. The results indicated that Nb<sub>0.05</sub>Ce<sub>0.05</sub>MnO<sub>x</sub> exhibited exceptional low-temperature performance, achieving over 90 % NO conversion at 125-250°C, along with significant resistance to K poisoning·NH<sub>3</sub>-TPD and <em>in-situ</em> experiments revealed that the loss of acid sites is the primary cause of K poisoning. The mechanism follows the L-H mechanism with L-acid sites as the main active sites on the catalyst surface and bridging nitrate as the key intermediate state. This research provides valuable insights into enhancing the industrial applicability of MnO<sub>x-</sub>based catalysts for low-temperature denitrification.\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"1 1\",\"pages\":\"\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2025-01-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.seppur.2025.131768\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.seppur.2025.131768","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Enhancing the K-resistance of MnOx catalysts via Ce and Nb co-doping for low-temperature NOx elimination
Manganese oxide (MnOx) catalysts are promising for low-temperature NH3-Selective Catalytic Reduction (NH3-SCR) with their superior catalytic performance. However, the presence of alkali metals in flue gases, particularly potassium (K), leads to catalyst deactivation and limits their industrial application. This study investigates the synergistic effects of Ce and Nb doping on the K resistance and low-temperature NH3-SCR activity of MnOx. The surface acidity and redox properties of MnOx were modulated by Ce and Nb modification. In addition, the phase structure, surface state and active sites of the catalysts were characterized before and after K poisoning. The results indicated that Nb0.05Ce0.05MnOx exhibited exceptional low-temperature performance, achieving over 90 % NO conversion at 125-250°C, along with significant resistance to K poisoning·NH3-TPD and in-situ experiments revealed that the loss of acid sites is the primary cause of K poisoning. The mechanism follows the L-H mechanism with L-acid sites as the main active sites on the catalyst surface and bridging nitrate as the key intermediate state. This research provides valuable insights into enhancing the industrial applicability of MnOx-based catalysts for low-temperature denitrification.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.