{"title":"cao掺杂铝负载Pd催化剂在甲醇分解中的优异性能","authors":"Busra Eryildirim, Nuray Oktar, Doruk Dogu","doi":"10.1007/s11164-025-05652-y","DOIUrl":null,"url":null,"abstract":"<div><p>This study aimed to investigate the impact of CaO incorporation to alumina-supported Pd catalysts on the methanol decomposition reaction. For this purpose, mayenite, alumina and/or calcium oxide-supported Pd catalysts were synthesized. The synthesized catalysts were characterized by XRD, FTIR, Laser Raman spectroscopy, N<sub>2</sub> adsorption–desorption, pyridine adsorbed DRIFTS, CO<sub>2</sub>-TPD, XPS, SEM–EDS, and ICP-OES techniques. Catalytic activity tests were carried out over a 6 h reaction period in the range of 100–400 °C. The results of the characterization and activity tests showed that the addition of CaO had significant effects on the physicochemical properties of the catalyst as well as on the catalytic activity. By adding CaO to the alumina support material, the acidity was reduced, thus reducing the selectivity for dimethyl ether (DME) formation, which is significantly high for the 1Pd@Al<sub>2</sub>O<sub>3</sub> catalyst, and increasing the H<sub>2</sub> and CO selectivity. The mayenite-supported catalyst (1Pd@SGM), which contains alumina and calcium oxide in its unique crystal structure, showed an excellent catalytic performance close to complete methanol conversion with DME selectivity below 1% at 400 °C. In the stability test carried out at 350 °C for 6 h with 1Pd@Al<sub>2</sub>O<sub>3</sub>, 1Pd@SGM, and 1Pd@48CaO@Al<sub>2</sub>O<sub>3</sub> catalysts used in the temperature scan, it was concluded that all catalysts were stable and 1Pd@SGM catalyst showed higher catalytic activity than the others.</p><h3>Graphical abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4149 - 4176"},"PeriodicalIF":3.5000,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11164-025-05652-y.pdf","citationCount":"0","resultStr":"{\"title\":\"Outperformance of CaO-incorporated alumina-supported Pd catalysts in methanol decomposition\",\"authors\":\"Busra Eryildirim, Nuray Oktar, Doruk Dogu\",\"doi\":\"10.1007/s11164-025-05652-y\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>This study aimed to investigate the impact of CaO incorporation to alumina-supported Pd catalysts on the methanol decomposition reaction. For this purpose, mayenite, alumina and/or calcium oxide-supported Pd catalysts were synthesized. The synthesized catalysts were characterized by XRD, FTIR, Laser Raman spectroscopy, N<sub>2</sub> adsorption–desorption, pyridine adsorbed DRIFTS, CO<sub>2</sub>-TPD, XPS, SEM–EDS, and ICP-OES techniques. Catalytic activity tests were carried out over a 6 h reaction period in the range of 100–400 °C. The results of the characterization and activity tests showed that the addition of CaO had significant effects on the physicochemical properties of the catalyst as well as on the catalytic activity. By adding CaO to the alumina support material, the acidity was reduced, thus reducing the selectivity for dimethyl ether (DME) formation, which is significantly high for the 1Pd@Al<sub>2</sub>O<sub>3</sub> catalyst, and increasing the H<sub>2</sub> and CO selectivity. The mayenite-supported catalyst (1Pd@SGM), which contains alumina and calcium oxide in its unique crystal structure, showed an excellent catalytic performance close to complete methanol conversion with DME selectivity below 1% at 400 °C. In the stability test carried out at 350 °C for 6 h with 1Pd@Al<sub>2</sub>O<sub>3</sub>, 1Pd@SGM, and 1Pd@48CaO@Al<sub>2</sub>O<sub>3</sub> catalysts used in the temperature scan, it was concluded that all catalysts were stable and 1Pd@SGM catalyst showed higher catalytic activity than the others.</p><h3>Graphical abstract</h3>\\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":753,\"journal\":{\"name\":\"Research on Chemical Intermediates\",\"volume\":\"51 8\",\"pages\":\"4149 - 4176\"},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2025-06-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://link.springer.com/content/pdf/10.1007/s11164-025-05652-y.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Research on Chemical Intermediates\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11164-025-05652-y\",\"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/s11164-025-05652-y","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Outperformance of CaO-incorporated alumina-supported Pd catalysts in methanol decomposition
This study aimed to investigate the impact of CaO incorporation to alumina-supported Pd catalysts on the methanol decomposition reaction. For this purpose, mayenite, alumina and/or calcium oxide-supported Pd catalysts were synthesized. The synthesized catalysts were characterized by XRD, FTIR, Laser Raman spectroscopy, N2 adsorption–desorption, pyridine adsorbed DRIFTS, CO2-TPD, XPS, SEM–EDS, and ICP-OES techniques. Catalytic activity tests were carried out over a 6 h reaction period in the range of 100–400 °C. The results of the characterization and activity tests showed that the addition of CaO had significant effects on the physicochemical properties of the catalyst as well as on the catalytic activity. By adding CaO to the alumina support material, the acidity was reduced, thus reducing the selectivity for dimethyl ether (DME) formation, which is significantly high for the 1Pd@Al2O3 catalyst, and increasing the H2 and CO selectivity. The mayenite-supported catalyst (1Pd@SGM), which contains alumina and calcium oxide in its unique crystal structure, showed an excellent catalytic performance close to complete methanol conversion with DME selectivity below 1% at 400 °C. In the stability test carried out at 350 °C for 6 h with 1Pd@Al2O3, 1Pd@SGM, and 1Pd@48CaO@Al2O3 catalysts used in the temperature scan, it was concluded that all catalysts were stable and 1Pd@SGM catalyst showed higher catalytic activity than the others.
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.
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