Suelen Martins Stutz Gomes, Samara da Silva Montani, Luz Amparo Palacio, Fatima Maria Zanon Zotin
{"title":"浸渍钾的铜铝催化剂在利用 CO 还原 NO 和 N2O 过程中的性能","authors":"Suelen Martins Stutz Gomes, Samara da Silva Montani, Luz Amparo Palacio, Fatima Maria Zanon Zotin","doi":"10.1016/j.cattod.2024.115140","DOIUrl":null,"url":null,"abstract":"<div><div>Three-way automotive catalysts (TWC) are based on noble metals and have two significant limitations: high cost and tendency to form, at low temperatures, nitrous oxide (N<sub>2</sub>O), which contributes to the greenhouse effect and ozone layer depletion. Thus, it is crucial to study possible substitutes for these components. In this work, catalysts prepared from copper and aluminum hydrotalcite-like materials impregnated with potassium were studied. The formation of the hydrotalcite phase and CuO phase in the catalyst was evidenced by X-ray diffraction (XRD). Temperature-programmed reduction (TPR) results showed that the alkali metal positively influences the reducibility of the catalyst, decreasing its reduction temperature. Temperature-programmed desorption (TPD) analysis revealed electronic promotion, confirming that the presence of potassium facilitates the desorption of molecular nitrogen from the surface and decreases that of N<sub>2</sub>O. Catalytic tests showed differences in the behavior of the catalysts depending on the pretreatment performed, suggesting that the interaction between potassium and oxidized or reduced copper gives rise to different catalytic sites. The formation of oxygen vacancies in potassium-containing catalysts, identified by XPS, and the increase in the copper metal surface area contributed to explaining the better performance of these catalysts. Also, based on the catalytic tests, more selective catalysts with the addition of potassium (minimizing N<sub>2</sub>O formation) were obtained, especially at a ratio of 0.025 K/Cu (mol/mol) and after a reducing pretreatment. This catalyst also showed 100 % N<sub>2</sub>O conversion in the reduction by CO at temperatures close to 100 °C, confirming its excellent performance in nitrous oxide abatement.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115140"},"PeriodicalIF":5.2000,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Performance of copper-aluminum catalysts impregnated with potassium in NO and N2O reduction by CO\",\"authors\":\"Suelen Martins Stutz Gomes, Samara da Silva Montani, Luz Amparo Palacio, Fatima Maria Zanon Zotin\",\"doi\":\"10.1016/j.cattod.2024.115140\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Three-way automotive catalysts (TWC) are based on noble metals and have two significant limitations: high cost and tendency to form, at low temperatures, nitrous oxide (N<sub>2</sub>O), which contributes to the greenhouse effect and ozone layer depletion. Thus, it is crucial to study possible substitutes for these components. In this work, catalysts prepared from copper and aluminum hydrotalcite-like materials impregnated with potassium were studied. The formation of the hydrotalcite phase and CuO phase in the catalyst was evidenced by X-ray diffraction (XRD). Temperature-programmed reduction (TPR) results showed that the alkali metal positively influences the reducibility of the catalyst, decreasing its reduction temperature. Temperature-programmed desorption (TPD) analysis revealed electronic promotion, confirming that the presence of potassium facilitates the desorption of molecular nitrogen from the surface and decreases that of N<sub>2</sub>O. Catalytic tests showed differences in the behavior of the catalysts depending on the pretreatment performed, suggesting that the interaction between potassium and oxidized or reduced copper gives rise to different catalytic sites. The formation of oxygen vacancies in potassium-containing catalysts, identified by XPS, and the increase in the copper metal surface area contributed to explaining the better performance of these catalysts. Also, based on the catalytic tests, more selective catalysts with the addition of potassium (minimizing N<sub>2</sub>O formation) were obtained, especially at a ratio of 0.025 K/Cu (mol/mol) and after a reducing pretreatment. This catalyst also showed 100 % N<sub>2</sub>O conversion in the reduction by CO at temperatures close to 100 °C, confirming its excellent performance in nitrous oxide abatement.</div></div>\",\"PeriodicalId\":264,\"journal\":{\"name\":\"Catalysis Today\",\"volume\":\"447 \",\"pages\":\"Article 115140\"},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2024-11-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Today\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0920586124006345\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Today","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0920586124006345","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Performance of copper-aluminum catalysts impregnated with potassium in NO and N2O reduction by CO
Three-way automotive catalysts (TWC) are based on noble metals and have two significant limitations: high cost and tendency to form, at low temperatures, nitrous oxide (N2O), which contributes to the greenhouse effect and ozone layer depletion. Thus, it is crucial to study possible substitutes for these components. In this work, catalysts prepared from copper and aluminum hydrotalcite-like materials impregnated with potassium were studied. The formation of the hydrotalcite phase and CuO phase in the catalyst was evidenced by X-ray diffraction (XRD). Temperature-programmed reduction (TPR) results showed that the alkali metal positively influences the reducibility of the catalyst, decreasing its reduction temperature. Temperature-programmed desorption (TPD) analysis revealed electronic promotion, confirming that the presence of potassium facilitates the desorption of molecular nitrogen from the surface and decreases that of N2O. Catalytic tests showed differences in the behavior of the catalysts depending on the pretreatment performed, suggesting that the interaction between potassium and oxidized or reduced copper gives rise to different catalytic sites. The formation of oxygen vacancies in potassium-containing catalysts, identified by XPS, and the increase in the copper metal surface area contributed to explaining the better performance of these catalysts. Also, based on the catalytic tests, more selective catalysts with the addition of potassium (minimizing N2O formation) were obtained, especially at a ratio of 0.025 K/Cu (mol/mol) and after a reducing pretreatment. This catalyst also showed 100 % N2O conversion in the reduction by CO at temperatures close to 100 °C, confirming its excellent performance in nitrous oxide abatement.
期刊介绍:
Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues.
Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.