The Influence of the Preparation Method on the Physico-Chemical Properties and Catalytic Activities of Ce-Modified LDH Structures Used as Catalysts in Condensation Reactions
Mechanical activation and mechanochemical reactions are the subjects of mechanochemistry, a special branch of chemistry studied intensively since the 19th century. Herein, we comparably describe two synthesis methods used to obtain the following layered double hydroxide doped with cerium, Mg<sub&...
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2021-10-01
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author | Alexandra-Elisabeta Stamate Rodica Zăvoianu Octavian Dumitru Pavel Ruxandra Birjega Andreea Matei Marius Dumitru Ioana Brezeștean Mariana Osiac Ioan-Cezar Marcu |
author_facet | Alexandra-Elisabeta Stamate Rodica Zăvoianu Octavian Dumitru Pavel Ruxandra Birjega Andreea Matei Marius Dumitru Ioana Brezeștean Mariana Osiac Ioan-Cezar Marcu |
author_sort | Alexandra-Elisabeta Stamate |
collection | DOAJ |
description | Mechanical activation and mechanochemical reactions are the subjects of mechanochemistry, a special branch of chemistry studied intensively since the 19th century. Herein, we comparably describe two synthesis methods used to obtain the following layered double hydroxide doped with cerium, Mg<sub>3</sub>Al<sub>0.75</sub>Ce<sub>0.25</sub>(OH)<sub>8</sub>(CO<sub>3</sub>)<sub>0.5</sub>·2H<sub>2</sub>O: the mechanochemical route and the co-precipitation method, respectively. The influence of the preparation method on the physico-chemical properties as determined by multiple techniques such as XRD, SEM, EDS, XPS, DRIFT, RAMAN, DR-UV-VIS, basicity, acidity, real/bulk densities, and BET measurements was also analyzed. The obtained samples, abbreviated HTCe-PP (prepared by co-precipitation) and HTCe-MC (prepared by mechanochemical method), and their corresponding mixed oxides, Ce-PP (resulting from HTCe-PP) and Ce-MC (resulting from HTCe-MC), were used as base catalysts in the self-condensation reaction of cyclohexanone and two Claisen–Schmidt condensations, which involve the reaction between an aromatic aldehyde and a ketone, at different molar ratios to synthesize compounds with significant biologic activity from the flavonoid family, namely chalcone (1,3-diphenyl-2-propen-1-one) and flavone (2-phenyl-4H-1benzoxiran-4-one). The mechanochemical route was shown to have indisputable advantages over the co-precipitation method for both the catalytic activity of the solids and the costs. |
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spelling | doaj.art-488fa60f2a4a46859792a2a2cd7ccd992023-11-22T19:19:32ZengMDPI AGMolecules1420-30492021-10-012620619110.3390/molecules26206191The Influence of the Preparation Method on the Physico-Chemical Properties and Catalytic Activities of Ce-Modified LDH Structures Used as Catalysts in Condensation ReactionsAlexandra-Elisabeta Stamate0Rodica Zăvoianu1Octavian Dumitru Pavel2Ruxandra Birjega3Andreea Matei4Marius Dumitru5Ioana Brezeștean6Mariana Osiac7Ioan-Cezar Marcu8Department of Organic Chemistry, Biochemistry and Catalysis, Faculty of Chemistry, University of Bucharest, 030018 Bucharest, RomaniaDepartment of Organic Chemistry, Biochemistry and Catalysis, Faculty of Chemistry, University of Bucharest, 030018 Bucharest, RomaniaDepartment of Organic Chemistry, Biochemistry and Catalysis, Faculty of Chemistry, University of Bucharest, 030018 Bucharest, RomaniaNational Institute for Lasers, Plasma and Radiation Physics, 077125 Magurele, RomaniaNational Institute for Lasers, Plasma and Radiation Physics, 077125 Magurele, RomaniaNational Institute for Lasers, Plasma and Radiation Physics, 077125 Magurele, RomaniaNational Institute for R&D of Isotopic and Molecular Technologies, 400293 Cluj-Napoca, RomaniaDepartment of Physics, INCESA, University of Craiova, 200585 Craiova, RomaniaDepartment of Organic Chemistry, Biochemistry and Catalysis, Faculty of Chemistry, University of Bucharest, 030018 Bucharest, RomaniaMechanical activation and mechanochemical reactions are the subjects of mechanochemistry, a special branch of chemistry studied intensively since the 19th century. Herein, we comparably describe two synthesis methods used to obtain the following layered double hydroxide doped with cerium, Mg<sub>3</sub>Al<sub>0.75</sub>Ce<sub>0.25</sub>(OH)<sub>8</sub>(CO<sub>3</sub>)<sub>0.5</sub>·2H<sub>2</sub>O: the mechanochemical route and the co-precipitation method, respectively. The influence of the preparation method on the physico-chemical properties as determined by multiple techniques such as XRD, SEM, EDS, XPS, DRIFT, RAMAN, DR-UV-VIS, basicity, acidity, real/bulk densities, and BET measurements was also analyzed. The obtained samples, abbreviated HTCe-PP (prepared by co-precipitation) and HTCe-MC (prepared by mechanochemical method), and their corresponding mixed oxides, Ce-PP (resulting from HTCe-PP) and Ce-MC (resulting from HTCe-MC), were used as base catalysts in the self-condensation reaction of cyclohexanone and two Claisen–Schmidt condensations, which involve the reaction between an aromatic aldehyde and a ketone, at different molar ratios to synthesize compounds with significant biologic activity from the flavonoid family, namely chalcone (1,3-diphenyl-2-propen-1-one) and flavone (2-phenyl-4H-1benzoxiran-4-one). The mechanochemical route was shown to have indisputable advantages over the co-precipitation method for both the catalytic activity of the solids and the costs.https://www.mdpi.com/1420-3049/26/20/6191layered double hydroxidesceriummechanochemicalco-precipitationcyclohexanone self-condensationClaisen–Schmidt condensation |
spellingShingle | Alexandra-Elisabeta Stamate Rodica Zăvoianu Octavian Dumitru Pavel Ruxandra Birjega Andreea Matei Marius Dumitru Ioana Brezeștean Mariana Osiac Ioan-Cezar Marcu The Influence of the Preparation Method on the Physico-Chemical Properties and Catalytic Activities of Ce-Modified LDH Structures Used as Catalysts in Condensation Reactions Molecules layered double hydroxides cerium mechanochemical co-precipitation cyclohexanone self-condensation Claisen–Schmidt condensation |
title | The Influence of the Preparation Method on the Physico-Chemical Properties and Catalytic Activities of Ce-Modified LDH Structures Used as Catalysts in Condensation Reactions |
title_full | The Influence of the Preparation Method on the Physico-Chemical Properties and Catalytic Activities of Ce-Modified LDH Structures Used as Catalysts in Condensation Reactions |
title_fullStr | The Influence of the Preparation Method on the Physico-Chemical Properties and Catalytic Activities of Ce-Modified LDH Structures Used as Catalysts in Condensation Reactions |
title_full_unstemmed | The Influence of the Preparation Method on the Physico-Chemical Properties and Catalytic Activities of Ce-Modified LDH Structures Used as Catalysts in Condensation Reactions |
title_short | The Influence of the Preparation Method on the Physico-Chemical Properties and Catalytic Activities of Ce-Modified LDH Structures Used as Catalysts in Condensation Reactions |
title_sort | influence of the preparation method on the physico chemical properties and catalytic activities of ce modified ldh structures used as catalysts in condensation reactions |
topic | layered double hydroxides cerium mechanochemical co-precipitation cyclohexanone self-condensation Claisen–Schmidt condensation |
url | https://www.mdpi.com/1420-3049/26/20/6191 |
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