{"title":"Fe3+ 或 Fe2+ 物种对经铁源改性的 CWK 在 NH3-SCR 反应中的催化性能和反应路径的影响","authors":"Ruihua Guo, Zhongxian Song, Xi Chen, Wei Liu, Mengru Zhang, Yehua Fan, Hongrun Gao, Haiyang Li, Xuejun Zhang","doi":"10.1007/s11164-024-05425-z","DOIUrl":null,"url":null,"abstract":"<div><p>Developing high-performance catalysts for NO<sub><i>x</i></sub> reduction was a significant challenge. CWK catalysts modified with iron sources were synthesized using co-precipitation and impregnation methods. The CWK-F<sub>3</sub>C and CWK-F<sub>3</sub>S catalysts exhibited the superior catalytic activity at 250–350 ℃ and the excellent N<sub>2</sub> selectivity. The key reasons for the enhanced catalytic activity of CWK-F<sub>3</sub>C and CWK-F<sub>3</sub>S catalysts could be attributed to the higher Fe<sup>3+</sup> concentration, more surface chemisorbed oxygen species and bigger relative fraction of Ce<sup>3+</sup>. More significantly, the adsorption of NH<sub>3</sub> and redox capability were both strengthened by the Fe<sup>3+</sup> doping. The DRIFTS experiment results showed that the E-R and L–H mechanism were followed by CWK-F<sub>3</sub>C and CWK-F<sub>2</sub>C catalysts. Furthermore, the introduction of Fe<sup>3+</sup> generated more surface acidic sites, which could facilitate the formation of key intermediates (-NH<sub>2</sub>) (NH<sub>3(ads)</sub> + O<sub>(ads)</sub>/O<sup>2−</sup>(ads) → -NH<sub>2(ads)</sub> + -OH<sub>(ads)</sub>). The presence of Fe<sup>3+</sup> was conducive to NO<sub>3</sub><sup>−</sup> formation (NO<sub>3</sub><sup>−</sup> + NO<sub>(ads)</sub> → NO<sub>2(ads)</sub>), resulting in the presence of fast reaction, causing the excellent low temperature catalytic performance. Hence, the production of -NH<sub>2</sub> and NO<sub>3</sub><sup>−</sup> species was responsible for the outstanding catalytic activity of CWK-F<sub>3</sub>C.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"50 12","pages":"5679 - 5697"},"PeriodicalIF":2.8000,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of Fe3+ or Fe2+ species on the catalytic performance and reaction pathway over CWK modified by iron sources in NH3-SCR reaction\",\"authors\":\"Ruihua Guo, Zhongxian Song, Xi Chen, Wei Liu, Mengru Zhang, Yehua Fan, Hongrun Gao, Haiyang Li, Xuejun Zhang\",\"doi\":\"10.1007/s11164-024-05425-z\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Developing high-performance catalysts for NO<sub><i>x</i></sub> reduction was a significant challenge. CWK catalysts modified with iron sources were synthesized using co-precipitation and impregnation methods. The CWK-F<sub>3</sub>C and CWK-F<sub>3</sub>S catalysts exhibited the superior catalytic activity at 250–350 ℃ and the excellent N<sub>2</sub> selectivity. The key reasons for the enhanced catalytic activity of CWK-F<sub>3</sub>C and CWK-F<sub>3</sub>S catalysts could be attributed to the higher Fe<sup>3+</sup> concentration, more surface chemisorbed oxygen species and bigger relative fraction of Ce<sup>3+</sup>. More significantly, the adsorption of NH<sub>3</sub> and redox capability were both strengthened by the Fe<sup>3+</sup> doping. The DRIFTS experiment results showed that the E-R and L–H mechanism were followed by CWK-F<sub>3</sub>C and CWK-F<sub>2</sub>C catalysts. Furthermore, the introduction of Fe<sup>3+</sup> generated more surface acidic sites, which could facilitate the formation of key intermediates (-NH<sub>2</sub>) (NH<sub>3(ads)</sub> + O<sub>(ads)</sub>/O<sup>2−</sup>(ads) → -NH<sub>2(ads)</sub> + -OH<sub>(ads)</sub>). The presence of Fe<sup>3+</sup> was conducive to NO<sub>3</sub><sup>−</sup> formation (NO<sub>3</sub><sup>−</sup> + NO<sub>(ads)</sub> → NO<sub>2(ads)</sub>), resulting in the presence of fast reaction, causing the excellent low temperature catalytic performance. Hence, the production of -NH<sub>2</sub> and NO<sub>3</sub><sup>−</sup> species was responsible for the outstanding catalytic activity of CWK-F<sub>3</sub>C.</p></div>\",\"PeriodicalId\":753,\"journal\":{\"name\":\"Research on Chemical Intermediates\",\"volume\":\"50 12\",\"pages\":\"5679 - 5697\"},\"PeriodicalIF\":2.8000,\"publicationDate\":\"2024-10-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Research on Chemical Intermediates\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11164-024-05425-z\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Research on Chemical Intermediates","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s11164-024-05425-z","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Effect of Fe3+ or Fe2+ species on the catalytic performance and reaction pathway over CWK modified by iron sources in NH3-SCR reaction
Developing high-performance catalysts for NOx reduction was a significant challenge. CWK catalysts modified with iron sources were synthesized using co-precipitation and impregnation methods. The CWK-F3C and CWK-F3S catalysts exhibited the superior catalytic activity at 250–350 ℃ and the excellent N2 selectivity. The key reasons for the enhanced catalytic activity of CWK-F3C and CWK-F3S catalysts could be attributed to the higher Fe3+ concentration, more surface chemisorbed oxygen species and bigger relative fraction of Ce3+. More significantly, the adsorption of NH3 and redox capability were both strengthened by the Fe3+ doping. The DRIFTS experiment results showed that the E-R and L–H mechanism were followed by CWK-F3C and CWK-F2C catalysts. Furthermore, the introduction of Fe3+ generated more surface acidic sites, which could facilitate the formation of key intermediates (-NH2) (NH3(ads) + O(ads)/O2−(ads) → -NH2(ads) + -OH(ads)). The presence of Fe3+ was conducive to NO3− formation (NO3− + NO(ads) → NO2(ads)), resulting in the presence of fast reaction, causing the excellent low temperature catalytic performance. Hence, the production of -NH2 and NO3− species was responsible for the outstanding catalytic activity of CWK-F3C.
期刊介绍:
Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry.
The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.