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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>
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>
Ivanchikova, Irina D.,Lee, Ji Sun,Maksimchuk, Nataliya V.,Shmakov, Alexander N.,Chesalov, Yurii A.,Ayupov, Artem B.,Hwang, Young Kyu,Jun, Chul‐,Ho,Chang, Jong‐,San,Kholdeeva, Oxana A. Wiley-VCH 2014 European journal of inorganic chemistry Vol. No.
<P><B>Abstract</B></P><P>The titanium‐based metal–organic framework MIL‐125 and its amine‐functionalized analog, MIL‐125_NH<SUB>2</SUB>, have been synthesized and characterized by elemental analysis, XRD, SEM, TEM, N<SUB>2</SUB> adsorption measurements, and spectroscopic techniques, including FTIR, Raman, and DR UV/Vis spectroscopy. Catalytic properties of MIL‐125 and MIL‐125_NH<SUB>2</SUB> were evaluated in the selective oxidation of two representative alkyl‐substituted phenols, 2,3,6‐trimethylphenol and 2,6‐di‐<I>tert</I>‐butylphenol, with the clean oxidant H<SUB>2</SUB>O<SUB>2</SUB>. With both MIL‐125 and MIL‐125_NH<SUB>2</SUB>, the selectivity toward the corresponding <I>p</I>‐benzoquinones was 100 %. Samples of MIL‐125 with different sizes of crystallites (0.5, 1.5, and 5 μm) demonstrated similar reaction rates, thus indicating the absence of diffusion limitations. The efficiency of the oxidant utilization and stability of the MIL‐125 structure increased upon decreasing the amount of water in the reaction mixture. Even if the structural integrity of MIL‐125 was destroyed by the reaction medium, the metal–organic framework acted as a precursor for the highly active, selective, and recyclable catalyst. The MIL‐125‐derived materials were stable toward titanium leaching, behaved as true heterogeneous catalysts, and could easily be recovered by filtration and reused several times without the loss of the catalytic properties.</P>
( A. S. Berdinsky ),( Yu. V. Shevtsov ),( Hui Gon Chun ),( Yong Zoo Yoo ),( D. Fink ),( B. M. Ayupov ) 한국센서학회 2004 센서학회지 Vol.13 No.5
We report on the technology of formation of sandwich structures based on fullerite films and on experimental results in research of optical and conductivity properties of these sandwich samples. Single crystals of sapphire (100) or silicon were used as substrates. The sandwich specimens were based on the structure M/C_(60)/M (M=Cr, Pd, Ag, Al, Cu). The thickness of the fullerite films was about 0.2~1.0 μm. The area of the C50 film under the top contact was about I cm². The specimens have been investigated by infrared spectroscopy, spectra-photometry. ellipsometry and X-ray diffraction analysis. Measurements of the current/voltage characteristics and research on the temperature dependence of conductivity were performed as well. It was shown that metals such as Cr, Pd. Ag. Al, and Cu penetrate easily into the fullerite films. It appears that these specimens have a large conductivity. For silver/C_(60) and other sandwich structures the conductivities show a semiconductor-like behaviour.