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Timofeeva, M. N.,Prikhod’ko, S. A.,Makarova, K. N.,Malyshev, M. E.,Panchenko, V. N.,Ayupov, A. B.,Jhung, S. H. Springer Science and Business Media 2017 Reaction kinetics, mechanisms and catalysis Vol.121 No.2
<P>The cyclocondensation of 1,2-phenylenediamine (I) with acetone was investigated in the presence of Fe-containing microporous nickel phosphate molecular sieves (Fe-VSB-5) and Fe-containing mesoporous mesophase materials (Fe-MMM). The main product was 2,3-dihydro-2,2,4-trimethyl-1H-1,5-benzodiazepine (1,5-benzodiazepine) with 86-88% yield at 50 degrees C, with an acetone/(I) molar ratio of 2.5 in methanol as the reaction medium. The Fe content was found to affect not only the reaction rate but also yield of 1,5-benzodiazepine. The high reaction rate and yield of 1,5-benzodiazepine were-achieved with isolated iron sites in frameworks of Fe-VSB-5 and Fe-MMM.</P>
Timofeeva, M.N.,Panchenko, V.N.,Prikhod'ko, S.A.,Ayupov, A.B.,Larichev, Yu.V.,Khan, Nazmul Abedin,Jhung, Sung Hwa Academic Press 2017 Journal of catalysis Vol.354 No.-
<P><B>Abstract</B></P> <P>Benzodiazepines and their derivatives are a very important class of nitrogen-containing heterocyclic compounds with biological activity that are widely used in medicine. In this study, we demonstrated synthesis of 1,5-benzodiazepines from 1,2-phenylenediamine and ketones (acetone, cyclohexanone, acetophenone, methyl ethyl ketone) in the presence of isostructural porous metal-benzenetricarboxylates of the families MIL-100(M) (M: V<SUP>3+</SUP>, Al<SUP>3+</SUP>, Fe<SUP>3+</SUP> and Cr<SUP>3+</SUP>) and three porous aluminium trimesates Al-BTCs (MIL-96(Al), MIL-100(Al) and MIL-110(Al)). A combination of catalytic, theoretical and physicochemical methods showed that reaction rates and yields of 1,5-benzodiazepines were adjusted by the type of metal ions and accessibility of active sites. The yield of 1,5-benzodiazepines in the presence of MIL-100(M) was comparable with zeolites, such as HY, H-ZSM−5, β-zeolite and heulandite.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Synthesis of 1,5-benzodiazepines over MIL-100(M), MIL-110 and MIL-96 was studied. </LI> <LI> Effect of Brønsted and Lewis acidity on MIL’s performance was investigated. </LI> <LI> Lewis acidity of MIL-100(Fe, Cr, Al, V) was studied by EPR spectroscopy. </LI> <LI> The type of M<SUP>3+</SUP>(Al, Fe, Cr, V) and structure of MILs affect the yield of product. </LI> <LI> MIL-100(M) samples perform well in compared with zeolites. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>
Panchenko, Valentina N.,Timofeeva, Maria N.,Jhung, Sung Hwa Taylor Francis 2016 Catalysis reviews: science and engineering Vol.58 No.2
<P>This article summarizes several approaches for understanding the catalytic chemistry and structure-surface acidity-reactivity relationships in a multiplicity of catalytic applications of a continually increasing assemblage of metal-organic frameworks (MOFs) structures. The various spectroscopic techniques for acid-base characterization of MOFs are reviewed. The experimental requirements and the type and nature of probe molecules available are also discussed. Special emphasis is given to the revealing of the surface acid-base effect on the catalytic performance of MOFs.</P>
Delidovich, Irina V.,Timofeeva, Maria N.,Orlov, Alexander Yu.,Panchenko, Valentina N.,Hasan, Zubair,Jhung, Sung Hwa,Taran, Oxana P.,Parmon, Valentin N. The Royal Society of Chemistry 2012 NEW JOURNAL OF CHEMISTRY Vol.36 No.11
<P>Condensation of dihydroxyacetone with formaldehyde was found to be effectively catalyzed by nickel phosphate molecular sieves (VSB-5 and Fe–VSB-5) in neutral aqueous medium. In the presence of VSB-5 the main products are erythrulose and 3-pentulose, while Fe–VSB-5 favours the formation of only erythrulose.</P> <P>Graphic Abstract</P><P>Condensation of dihydroxyacetone with formaldehyde was found to be effectively catalyzed by nickel phosphate molecular sieves (VSB-5 and Fe–VSB-5) in neutral aqueous medium. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c2nj40363c'> </P>
Kozlova, Ekaterina A.,Panchenko, Valentina N.,Hasan, Zubair,Khan, Namzul Abedin,Timofeeva, Maria N.,Jhung, Sung Hwa Elsevier 2016 CATALYSIS TODAY - Vol.266 No.-
<P><B>Abstract</B></P> <P>The effect of metal ions and functional groups in organic ligands on the photocatalytic properties of metal-carboxylates, such as isostructural MIL-100(M) (M=Al, Fe, V, and Cr), isoreticular UiO-66-R (R=H, NH<SUB>2</SUB>, and NO<SUB>2</SUB>), MIL-47(V), and MIL-125(Ti), was investigated using the decolorization of methylene blue in aqueous solution at pH 7.0 and 20°C under UV radiation. The metal-carboxylates were characterized by diffuse reflectance UV/vis measurements. The determination of the band gap (<I>E</I> <SUB> <I>g</I> </SUB>) on the basis of DR-UV/vis measurements showed that <I>E</I> <SUB> <I>g</I> </SUB> values correlate with ionic covalent parameters, i.e., the strength of the interaction between metal and oxygen in the “M<SUP>+<I>n</I> </SUP>-O<SUP>2−</SUP> pair. According to DR-UV/vis spectroscopic and catalytic investigations, the reactivity of metal-carboxylates correlated with the band-gap value (<I>E</I> <SUB> <I>g</I> </SUB>), which could be adjusted by varying the nature of the metal ions in SBUs or functional groups in the organic ligands.</P> <P><B>Highlights</B></P> <P> <UL> <LI> The photocatalytic decolorization of methylene blue dye in aqueous solution was studied. </LI> <LI> Isostructural MIL-100(M) (M=Al, Fe, V and Cr) materials were used as photocatalysts. </LI> <LI> Reactivity of isostructural MIL-100(M) materials depends on the type of metal ions. </LI> <LI> Isoreticular UiO-66-R (H, NH<SUB>2</SUB> and NO<SUB>2</SUB>) materials were used as photocatalysts. </LI> <LI> Reactivity of isoreticular UiO-66-R materials depends on the functional groups in organic ligands. </LI> </UL> </P>