Kaiwei Qin, Lei Guo, Shujun Ming, Shoute Zhang, Yanbin Guo, Lei Pang, Tao Li
{"title":"Cu-SSZ-13与Fe-SSZ-13对NH3-SCR反应机理及催化性能的比较研究","authors":"Kaiwei Qin, Lei Guo, Shujun Ming, Shoute Zhang, Yanbin Guo, Lei Pang, Tao Li","doi":"10.1007/s10563-022-09353-z","DOIUrl":null,"url":null,"abstract":"<div><p>The catalytic performances and mechanism differences of model catalysts Cu–SSZ-13 and Fe–SSZ-13 with similar metal content and Si/Al ratio were compared. In the NH<sub>3</sub>-SCR reaction, Cu–SSZ-13 had a good NO conversion at low temperature, broad active temperature windows and better hydrothermal stability. Fe–SSZ-13 showed better high-temperature NO conversion rate and better resistance to sulfur poisoning, but poorer low-temperature NH<sub>3</sub>-SCR activity. NH<sub>3</sub>-TPD verified the content difference of L-NH<sub>3</sub> and B-NH<sub>3</sub> of Cu- and Fe–SSZ-13. UV–Vis DRS, EPR, H<sub>2</sub>-TPR indicated the active species of Cu- and Fe–SSZ-13. Results showed that Cu–SSZ-13 only had one type active species of Cu<sup>2+</sup>, Fe–SSZ-13 had Fe<sup>3+</sup> species that acted as active centers at low temperature and reactivity oligomeric Fe species at high temperature. The diffuse reflection infrared Fourier transform spectrum (DRIFTS) results showed that the reactions of Cu–SSZ-13 and Fe–SSZ-13 at low temperature both followed the Eley–Rideal (E–R) mechanism and the Langmuir–Hinshelwood (L–H) mechanism. Cu–SSZ-13 could perform the catalytic process well under both mechanisms, but when Fe–SSZ-13 followed the E–R mechanism, there were many B-NH<sub>3</sub> species, which was not conducive to the reaction. When following the L–H mechanism, the speed of NO<sub>3</sub><sup>−</sup> participating in the reaction was slow due to ammonia inhibition, resulting in poor low-temperature activity.</p></div>","PeriodicalId":509,"journal":{"name":"Catalysis Surveys from Asia","volume":"26 2","pages":"115 - 128"},"PeriodicalIF":2.1000,"publicationDate":"2022-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"6","resultStr":"{\"title\":\"The Comparative Study of Reaction Mechanisms and Catalytic Performances of Cu–SSZ-13 and Fe–SSZ-13 for the NH3-SCR Reaction\",\"authors\":\"Kaiwei Qin, Lei Guo, Shujun Ming, Shoute Zhang, Yanbin Guo, Lei Pang, Tao Li\",\"doi\":\"10.1007/s10563-022-09353-z\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The catalytic performances and mechanism differences of model catalysts Cu–SSZ-13 and Fe–SSZ-13 with similar metal content and Si/Al ratio were compared. In the NH<sub>3</sub>-SCR reaction, Cu–SSZ-13 had a good NO conversion at low temperature, broad active temperature windows and better hydrothermal stability. Fe–SSZ-13 showed better high-temperature NO conversion rate and better resistance to sulfur poisoning, but poorer low-temperature NH<sub>3</sub>-SCR activity. NH<sub>3</sub>-TPD verified the content difference of L-NH<sub>3</sub> and B-NH<sub>3</sub> of Cu- and Fe–SSZ-13. UV–Vis DRS, EPR, H<sub>2</sub>-TPR indicated the active species of Cu- and Fe–SSZ-13. Results showed that Cu–SSZ-13 only had one type active species of Cu<sup>2+</sup>, Fe–SSZ-13 had Fe<sup>3+</sup> species that acted as active centers at low temperature and reactivity oligomeric Fe species at high temperature. The diffuse reflection infrared Fourier transform spectrum (DRIFTS) results showed that the reactions of Cu–SSZ-13 and Fe–SSZ-13 at low temperature both followed the Eley–Rideal (E–R) mechanism and the Langmuir–Hinshelwood (L–H) mechanism. Cu–SSZ-13 could perform the catalytic process well under both mechanisms, but when Fe–SSZ-13 followed the E–R mechanism, there were many B-NH<sub>3</sub> species, which was not conducive to the reaction. When following the L–H mechanism, the speed of NO<sub>3</sub><sup>−</sup> participating in the reaction was slow due to ammonia inhibition, resulting in poor low-temperature activity.</p></div>\",\"PeriodicalId\":509,\"journal\":{\"name\":\"Catalysis Surveys from Asia\",\"volume\":\"26 2\",\"pages\":\"115 - 128\"},\"PeriodicalIF\":2.1000,\"publicationDate\":\"2022-02-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"6\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Surveys from Asia\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10563-022-09353-z\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Surveys from Asia","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10563-022-09353-z","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
The Comparative Study of Reaction Mechanisms and Catalytic Performances of Cu–SSZ-13 and Fe–SSZ-13 for the NH3-SCR Reaction
The catalytic performances and mechanism differences of model catalysts Cu–SSZ-13 and Fe–SSZ-13 with similar metal content and Si/Al ratio were compared. In the NH3-SCR reaction, Cu–SSZ-13 had a good NO conversion at low temperature, broad active temperature windows and better hydrothermal stability. Fe–SSZ-13 showed better high-temperature NO conversion rate and better resistance to sulfur poisoning, but poorer low-temperature NH3-SCR activity. NH3-TPD verified the content difference of L-NH3 and B-NH3 of Cu- and Fe–SSZ-13. UV–Vis DRS, EPR, H2-TPR indicated the active species of Cu- and Fe–SSZ-13. Results showed that Cu–SSZ-13 only had one type active species of Cu2+, Fe–SSZ-13 had Fe3+ species that acted as active centers at low temperature and reactivity oligomeric Fe species at high temperature. The diffuse reflection infrared Fourier transform spectrum (DRIFTS) results showed that the reactions of Cu–SSZ-13 and Fe–SSZ-13 at low temperature both followed the Eley–Rideal (E–R) mechanism and the Langmuir–Hinshelwood (L–H) mechanism. Cu–SSZ-13 could perform the catalytic process well under both mechanisms, but when Fe–SSZ-13 followed the E–R mechanism, there were many B-NH3 species, which was not conducive to the reaction. When following the L–H mechanism, the speed of NO3− participating in the reaction was slow due to ammonia inhibition, resulting in poor low-temperature activity.
期刊介绍:
Early dissemination of important findings from Asia which may lead to new concepts in catalyst design is the main aim of this journal. Rapid, invited, short reviews and perspectives from academia and industry will constitute the major part of Catalysis Surveys from Asia . Surveys of recent progress and activities in catalytic science and technology and related areas in Asia will be covered regularly as well. We would appreciate critical comments from colleagues throughout the world about articles in Catalysis Surveys from Asia . If requested and thought appropriate, the comments will be included in the journal. We will be very happy if this journal stimulates global communication between scientists and engineers in the world of catalysis.