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&...

Full description

Bibliographic Details
Main Authors: Alexandra-Elisabeta Stamate, Rodica Zăvoianu, Octavian Dumitru Pavel, Ruxandra Birjega, Andreea Matei, Marius Dumitru, Ioana Brezeștean, Mariana Osiac, Ioan-Cezar Marcu
Format: Article
Language:English
Published: MDPI AG 2021-10-01
Series:Molecules
Subjects:
Online Access:https://www.mdpi.com/1420-3049/26/20/6191
_version_ 1797513681298259968
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.
first_indexed 2024-03-10T06:20:58Z
format Article
id doaj.art-488fa60f2a4a46859792a2a2cd7ccd99
institution Directory Open Access Journal
issn 1420-3049
language English
last_indexed 2024-03-10T06:20:58Z
publishDate 2021-10-01
publisher MDPI AG
record_format Article
series Molecules
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
work_keys_str_mv AT alexandraelisabetastamate theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT rodicazavoianu theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT octaviandumitrupavel theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT ruxandrabirjega theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT andreeamatei theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT mariusdumitru theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT ioanabrezestean theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT marianaosiac theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT ioancezarmarcu theinfluenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT alexandraelisabetastamate influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT rodicazavoianu influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT octaviandumitrupavel influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT ruxandrabirjega influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT andreeamatei influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT mariusdumitru influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT ioanabrezestean influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT marianaosiac influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions
AT ioancezarmarcu influenceofthepreparationmethodonthephysicochemicalpropertiesandcatalyticactivitiesofcemodifiedldhstructuresusedascatalystsincondensationreactions