{"title":"调节MMoOx (M = Mn, Fe, Cr)催化剂的氧化还原位点对NH3的高效选择性催化氧化","authors":"Lan Hu, Qiuyue Zhao, Xinling Zhang, Huipeng Li, Cheng Bian, Yiqing Zeng","doi":"10.1007/s11164-025-05651-z","DOIUrl":null,"url":null,"abstract":"<div><p>Redox sites and acidic sites are the main active sites of bimetallic oxide catalysts used for selective catalytic oxidation of NH<sub>3</sub> (NH<sub>3</sub>-SCO). In this work, three MMoO<i>x</i> (M = Cr, Fe, and Mn) bimetallic oxides catalysts were prepared by simple grinding and calcination to investigate the effect of redox sites (M sites) on the NH<sub>3</sub>-SCO performance. The NH<sub>3</sub>-SCO test results showed that the activity of MMoO<i>x</i> is in the order of CrMoO<i>x</i> > MnMoO<i>x</i> > FeMoO<i>x</i>. The characterization results of H<sub>2</sub>-TPR, O<sub>2</sub>-TPD, NH<sub>3</sub>-TPD, and in situ DRIFTS proposed that the NH<sub>3</sub>-SCO reaction on MMoO<i>x</i> catalysts is proceed via i-SCR mechanism, and the formation of the intermediates of NH<sub>3</sub>-SCR reaction is the decisive reaction step. Owing to the excellent ability in promoting the formation of nitrate/nitrite species, CrMoO<sub><i>x</i></sub> and MnMoO<i>x</i> samples show much higher NH<sub>3</sub>-SCO activity than FeMoO<i>x</i> sample<i>.</i> CrMoO<sub><i>x</i></sub> can facilitate the formation of a large amount of –NH<sub>2</sub> species, which together with nitrate/nitrite species enhance the NH<sub>3</sub>-SCO reaction via i-SCR reaction route. Therefore, CrMoO<sub><i>x</i></sub> shows the highest NH<sub>3</sub>-SCO activity among the MMoO<i>x</i> catalysts. Through this work, the redox sites of bimetallic oxide catalysts are demonstrated as a vital role in inducing the formation of reaction-active intermediates, which highlight the importance of choosing the redox sites in designing NH<sub>3</sub>-SCO catalyst.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4177 - 4190"},"PeriodicalIF":3.5000,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Regulating the redox sites of MMoOx (M = Mn, Fe, Cr) catalysts for highly efficient selective catalytic oxidation of NH3\",\"authors\":\"Lan Hu, Qiuyue Zhao, Xinling Zhang, Huipeng Li, Cheng Bian, Yiqing Zeng\",\"doi\":\"10.1007/s11164-025-05651-z\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Redox sites and acidic sites are the main active sites of bimetallic oxide catalysts used for selective catalytic oxidation of NH<sub>3</sub> (NH<sub>3</sub>-SCO). In this work, three MMoO<i>x</i> (M = Cr, Fe, and Mn) bimetallic oxides catalysts were prepared by simple grinding and calcination to investigate the effect of redox sites (M sites) on the NH<sub>3</sub>-SCO performance. The NH<sub>3</sub>-SCO test results showed that the activity of MMoO<i>x</i> is in the order of CrMoO<i>x</i> > MnMoO<i>x</i> > FeMoO<i>x</i>. The characterization results of H<sub>2</sub>-TPR, O<sub>2</sub>-TPD, NH<sub>3</sub>-TPD, and in situ DRIFTS proposed that the NH<sub>3</sub>-SCO reaction on MMoO<i>x</i> catalysts is proceed via i-SCR mechanism, and the formation of the intermediates of NH<sub>3</sub>-SCR reaction is the decisive reaction step. Owing to the excellent ability in promoting the formation of nitrate/nitrite species, CrMoO<sub><i>x</i></sub> and MnMoO<i>x</i> samples show much higher NH<sub>3</sub>-SCO activity than FeMoO<i>x</i> sample<i>.</i> CrMoO<sub><i>x</i></sub> can facilitate the formation of a large amount of –NH<sub>2</sub> species, which together with nitrate/nitrite species enhance the NH<sub>3</sub>-SCO reaction via i-SCR reaction route. Therefore, CrMoO<sub><i>x</i></sub> shows the highest NH<sub>3</sub>-SCO activity among the MMoO<i>x</i> catalysts. Through this work, the redox sites of bimetallic oxide catalysts are demonstrated as a vital role in inducing the formation of reaction-active intermediates, which highlight the importance of choosing the redox sites in designing NH<sub>3</sub>-SCO catalyst.</p></div>\",\"PeriodicalId\":753,\"journal\":{\"name\":\"Research on Chemical Intermediates\",\"volume\":\"51 8\",\"pages\":\"4177 - 4190\"},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2025-06-26\",\"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/s11164-025-05651-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/s11164-025-05651-z","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Regulating the redox sites of MMoOx (M = Mn, Fe, Cr) catalysts for highly efficient selective catalytic oxidation of NH3
Redox sites and acidic sites are the main active sites of bimetallic oxide catalysts used for selective catalytic oxidation of NH3 (NH3-SCO). In this work, three MMoOx (M = Cr, Fe, and Mn) bimetallic oxides catalysts were prepared by simple grinding and calcination to investigate the effect of redox sites (M sites) on the NH3-SCO performance. The NH3-SCO test results showed that the activity of MMoOx is in the order of CrMoOx > MnMoOx > FeMoOx. The characterization results of H2-TPR, O2-TPD, NH3-TPD, and in situ DRIFTS proposed that the NH3-SCO reaction on MMoOx catalysts is proceed via i-SCR mechanism, and the formation of the intermediates of NH3-SCR reaction is the decisive reaction step. Owing to the excellent ability in promoting the formation of nitrate/nitrite species, CrMoOx and MnMoOx samples show much higher NH3-SCO activity than FeMoOx sample. CrMoOx can facilitate the formation of a large amount of –NH2 species, which together with nitrate/nitrite species enhance the NH3-SCO reaction via i-SCR reaction route. Therefore, CrMoOx shows the highest NH3-SCO activity among the MMoOx catalysts. Through this work, the redox sites of bimetallic oxide catalysts are demonstrated as a vital role in inducing the formation of reaction-active intermediates, which highlight the importance of choosing the redox sites in designing NH3-SCO catalyst.
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.