Zhiying Liu , Meiqing Shen , Shuhuan Wang , Chunjuan Zhang , Gurong Shen , Xinhua Li , Wei Li , Feng Gao
{"title":"CeO2/H-SSZ-13复合NH3-SCR催化剂实现了前所未有的高温N2选择性","authors":"Zhiying Liu , Meiqing Shen , Shuhuan Wang , Chunjuan Zhang , Gurong Shen , Xinhua Li , Wei Li , Feng Gao","doi":"10.1016/j.jcat.2025.116459","DOIUrl":null,"url":null,"abstract":"<div><div>A series of CeO<sub>2</sub>/H-SSZ-13 composite catalysts with CeO<sub>2</sub> contents ranging from 5 to 50 wt% are investigated. The catalysts are characterized using various techniques, including XRD, SEM, TEM, XPS, H<sub>2</sub>-TPR, Raman spectroscopy and chemical titrations coupled with TPD and DRIFTS. Their catalytic performance is evaluated through steady-state NH<sub>3</sub>-SCR. DFT calculations are also applied to supplement experimental data. The results demonstrate that the synergistic interactions between the redox domain (CeO<sub>2</sub>) and the acid domain (H-SSZ-13) render the composite catalysts with excellent medium-to-high-temperature deNO<sub>x</sub> efficiency. Notably, the formation of the unwanted N<sub>2</sub>O side product is completely eliminated over these composite catalysts. By systematically regulating redox and acid functions, it is revealed that CeO<sub>2</sub> serves as the key active component for the rate-determining NO activation step, while H-SSZ-13 facilitates NH<sub>3</sub> adsorption and the decomposition of reactive intermediates. Based on detailed studies of SCR kinetics, N<sub>2</sub>O formation, chemical trapping, as well as DFT calculations, it is proposed that the gaseous nitrite precursor HONO acts as the key reaction intermediate.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"453 ","pages":"Article 116459"},"PeriodicalIF":6.5000,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"CeO2/H-SSZ-13 composite NH3-SCR catalysts achieve unprecedented high-temperature N2 selectivity\",\"authors\":\"Zhiying Liu , Meiqing Shen , Shuhuan Wang , Chunjuan Zhang , Gurong Shen , Xinhua Li , Wei Li , Feng Gao\",\"doi\":\"10.1016/j.jcat.2025.116459\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>A series of CeO<sub>2</sub>/H-SSZ-13 composite catalysts with CeO<sub>2</sub> contents ranging from 5 to 50 wt% are investigated. The catalysts are characterized using various techniques, including XRD, SEM, TEM, XPS, H<sub>2</sub>-TPR, Raman spectroscopy and chemical titrations coupled with TPD and DRIFTS. Their catalytic performance is evaluated through steady-state NH<sub>3</sub>-SCR. DFT calculations are also applied to supplement experimental data. The results demonstrate that the synergistic interactions between the redox domain (CeO<sub>2</sub>) and the acid domain (H-SSZ-13) render the composite catalysts with excellent medium-to-high-temperature deNO<sub>x</sub> efficiency. Notably, the formation of the unwanted N<sub>2</sub>O side product is completely eliminated over these composite catalysts. By systematically regulating redox and acid functions, it is revealed that CeO<sub>2</sub> serves as the key active component for the rate-determining NO activation step, while H-SSZ-13 facilitates NH<sub>3</sub> adsorption and the decomposition of reactive intermediates. Based on detailed studies of SCR kinetics, N<sub>2</sub>O formation, chemical trapping, as well as DFT calculations, it is proposed that the gaseous nitrite precursor HONO acts as the key reaction intermediate.</div></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":\"453 \",\"pages\":\"Article 116459\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2025-10-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951725005251\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951725005251","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
A series of CeO2/H-SSZ-13 composite catalysts with CeO2 contents ranging from 5 to 50 wt% are investigated. The catalysts are characterized using various techniques, including XRD, SEM, TEM, XPS, H2-TPR, Raman spectroscopy and chemical titrations coupled with TPD and DRIFTS. Their catalytic performance is evaluated through steady-state NH3-SCR. DFT calculations are also applied to supplement experimental data. The results demonstrate that the synergistic interactions between the redox domain (CeO2) and the acid domain (H-SSZ-13) render the composite catalysts with excellent medium-to-high-temperature deNOx efficiency. Notably, the formation of the unwanted N2O side product is completely eliminated over these composite catalysts. By systematically regulating redox and acid functions, it is revealed that CeO2 serves as the key active component for the rate-determining NO activation step, while H-SSZ-13 facilitates NH3 adsorption and the decomposition of reactive intermediates. Based on detailed studies of SCR kinetics, N2O formation, chemical trapping, as well as DFT calculations, it is proposed that the gaseous nitrite precursor HONO acts as the key reaction intermediate.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.