Li Xu, Xingdong Zhu, Qiong Zhang, Xinyan Zhang, Xin Zhang
{"title":"NH3在MnCeOx/Cu-SSZ-39复合催化剂上有效选择性催化还原NOx:提高低温活性和水热稳定性","authors":"Li Xu, Xingdong Zhu, Qiong Zhang, Xinyan Zhang, Xin Zhang","doi":"10.1002/slct.202501205","DOIUrl":null,"url":null,"abstract":"<p>In this study, a composite catalyst, MnCeO<sub>x</sub>/Cu-SSZ-39, was synthesized by coupling MnCeO<sub>x</sub> with Cu-SSZ-39 zeolite and evaluated for NH<sub>3</sub>-SCR (selective catalytic reduction by NH<sub>3</sub>) performance. The incorporation of MnCeO<sub>x</sub> significantly enhanced the low-temperature SCR activity of Cu-SSZ-39 and broadened its operating temperature window. This improvement was attributed to the increased surface chemisorbed oxygen with high mobility, which facilitated NO oxidation to NO<sub>2</sub>, thereby promoting the fast SCR pathway and enhancing low-temperature activity. Furthermore, the hybrid catalyst exhibited higher concentrations of isolated Cu<sup>2</sup>⁺ and Ce<sup>3+</sup>/Mn<sup>4+</sup> species, improving redox capacity and surface acidity, both critical for low-temperature SCR reactions. Notably, MnCeO<sub>x</sub>/Cu-SSZ-39 demonstrated superior hydrothermal stability compared to pure Cu-SSZ-39, maintaining higher SCR activity after aging. Mechanistic studies revealed a strong metal oxide-zeolite interaction, where MnCeO<sub>x</sub> stabilized the zeolite framework, suppressed dealumination, and prevented Cu species aggregation during hydrothermal aging. These findings provide a promising strategy for designing Cu-SSZ-39 catalysts with excellent low-temperature activity, broad-temperature performance, and enhanced hydrothermal stability.</p>","PeriodicalId":146,"journal":{"name":"ChemistrySelect","volume":"10 25","pages":""},"PeriodicalIF":2.0000,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effective Selective Catalytic Reduction of NOx with NH3 over MnCeOx/Cu-SSZ-39 Composite Catalyst: Improved Low Temperature Activity and Hydrothermal Stability\",\"authors\":\"Li Xu, Xingdong Zhu, Qiong Zhang, Xinyan Zhang, Xin Zhang\",\"doi\":\"10.1002/slct.202501205\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>In this study, a composite catalyst, MnCeO<sub>x</sub>/Cu-SSZ-39, was synthesized by coupling MnCeO<sub>x</sub> with Cu-SSZ-39 zeolite and evaluated for NH<sub>3</sub>-SCR (selective catalytic reduction by NH<sub>3</sub>) performance. The incorporation of MnCeO<sub>x</sub> significantly enhanced the low-temperature SCR activity of Cu-SSZ-39 and broadened its operating temperature window. This improvement was attributed to the increased surface chemisorbed oxygen with high mobility, which facilitated NO oxidation to NO<sub>2</sub>, thereby promoting the fast SCR pathway and enhancing low-temperature activity. Furthermore, the hybrid catalyst exhibited higher concentrations of isolated Cu<sup>2</sup>⁺ and Ce<sup>3+</sup>/Mn<sup>4+</sup> species, improving redox capacity and surface acidity, both critical for low-temperature SCR reactions. Notably, MnCeO<sub>x</sub>/Cu-SSZ-39 demonstrated superior hydrothermal stability compared to pure Cu-SSZ-39, maintaining higher SCR activity after aging. Mechanistic studies revealed a strong metal oxide-zeolite interaction, where MnCeO<sub>x</sub> stabilized the zeolite framework, suppressed dealumination, and prevented Cu species aggregation during hydrothermal aging. These findings provide a promising strategy for designing Cu-SSZ-39 catalysts with excellent low-temperature activity, broad-temperature performance, and enhanced hydrothermal stability.</p>\",\"PeriodicalId\":146,\"journal\":{\"name\":\"ChemistrySelect\",\"volume\":\"10 25\",\"pages\":\"\"},\"PeriodicalIF\":2.0000,\"publicationDate\":\"2025-06-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ChemistrySelect\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/slct.202501205\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ChemistrySelect","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/slct.202501205","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Effective Selective Catalytic Reduction of NOx with NH3 over MnCeOx/Cu-SSZ-39 Composite Catalyst: Improved Low Temperature Activity and Hydrothermal Stability
In this study, a composite catalyst, MnCeOx/Cu-SSZ-39, was synthesized by coupling MnCeOx with Cu-SSZ-39 zeolite and evaluated for NH3-SCR (selective catalytic reduction by NH3) performance. The incorporation of MnCeOx significantly enhanced the low-temperature SCR activity of Cu-SSZ-39 and broadened its operating temperature window. This improvement was attributed to the increased surface chemisorbed oxygen with high mobility, which facilitated NO oxidation to NO2, thereby promoting the fast SCR pathway and enhancing low-temperature activity. Furthermore, the hybrid catalyst exhibited higher concentrations of isolated Cu2⁺ and Ce3+/Mn4+ species, improving redox capacity and surface acidity, both critical for low-temperature SCR reactions. Notably, MnCeOx/Cu-SSZ-39 demonstrated superior hydrothermal stability compared to pure Cu-SSZ-39, maintaining higher SCR activity after aging. Mechanistic studies revealed a strong metal oxide-zeolite interaction, where MnCeOx stabilized the zeolite framework, suppressed dealumination, and prevented Cu species aggregation during hydrothermal aging. These findings provide a promising strategy for designing Cu-SSZ-39 catalysts with excellent low-temperature activity, broad-temperature performance, and enhanced hydrothermal stability.
期刊介绍:
ChemistrySelect is the latest journal from ChemPubSoc Europe and Wiley-VCH. It offers researchers a quality society-owned journal in which to publish their work in all areas of chemistry. Manuscripts are evaluated by active researchers to ensure they add meaningfully to the scientific literature, and those accepted are processed quickly to ensure rapid online publication.