30 results on '"Pavel S. Yaremov"'
Search Results
2. Air-Stable Efficient Nickel Catalyst for Hydrogenation of Organic Compounds
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Vladyslav V. Subotin, Mykyta O. Ivanytsya, Anastasiya V. Terebilenko, Pavel S. Yaremov, Olena O. Pariiska, Yuri M. Akimov, Igor E. Kotenko, Tomash M. Sabov, Mykhailo M. Kurmach, Sergey V. Ryabukhin, Dmitriy M. Volochnyuk, and Sergey V. Kolotilov
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nickel ,composite ,catalysis ,hydrogenation ,hydrogen ,cyclooctadienyl ,Physical and Theoretical Chemistry ,Catalysis ,General Environmental Science - Abstract
A series of composites containing nanoparticles of NiO (from 1 to 10% by weight per Ni), deposited on NORIT charcoal, was prepared by the decomposition of the Ni0 complex Ni(cod)2 (cod = cis,cis-1,5-cyclooctadiene). Ni content in the composites was set by loading the appropriate quantities of the Ni(cod)2 precursor. The catalytic activity of the composites was associated with the in situ generation of active sites due to a reduction in NiO, hence the composites could be stored in air without a loss in their catalytic performance. The composites were analyzed by powder XRD, TEM, XPS, and adsorption methods. The hydrogenation of quinoline was used as a reference reaction for studies of the influence of temperature, P(H2), catalyst loading on the product yield, and for the selection of the composite possessing the highest performance. It was found that 3% Ni loading was the most optimal. This composite was used as an efficient catalyst for the hydrogenation of compounds with ethylene and acetylene bonds, nitro- and keto- groups as well as a series of substituted quinolines and analogs. The studied composites can be proposed as air-stable and efficient catalysts for the hydrogenation of a wide range of organic compounds.
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- 2023
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3. Hierarchical Beta zeolites as catalysts in a one-pot three-component cascade Prins–Friedel–Crafts reaction
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Roman Barakov, Maksym Opanasenko, Igor Bezverkhyy, Pavel S. Yaremov, Jiří Čejka, Nataliya D. Shcherban, Laboratoire Interdisciplinaire Carnot de Bourgogne [Dijon] (LICB), and Université de Bourgogne (UB)-Université de Technologie de Belfort-Montbeliard (UTBM)-Centre National de la Recherche Scientifique (CNRS)
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010405 organic chemistry ,Ether ,010402 general chemistry ,Anisole ,01 natural sciences ,Pollution ,Environmentally friendly ,0104 chemical sciences ,Catalysis ,[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry ,chemistry.chemical_compound ,Adsorption ,chemistry ,Environmental Chemistry ,Organic chemistry ,Butyraldehyde ,Brønsted–Lowry acid–base theory ,Friedel–Crafts reaction ,ComputingMilieux_MISCELLANEOUS - Abstract
Hierarchical Beta zeolites obtained from concentrated reaction mixtures (H2O/Si = 2.5–7.0) in the presence of CTAB and their conventional and nanosponge analogues were investigated in a one-pot cascade environmentally friendly Prins–Friedel–Crafts reaction of butyraldehyde with 3-buten-1-ol and anisole under mild conditions (60 °C). The highest yields of the desired products with 4-aryltetrahydropyran structure were achieved when using hierarchical zeolites characterised by well-developed mesoporosity (facilitating the formation of bulky intermediates and products) and by an increased fraction of highly accessible (evaluated by TTBPy method) medium-strength Bronsted acid sites. Acid sites with higher strength promote strong adsorption of bulk O-containing intermediates or products and the formation of byproducts (tetrahydropyranyl ether and 2-propyloxan-4-ol). Therefore, this is an inexpensive and simple synthesis method for preparing hierarchical zeolites with catalytic activity comparable to that of nanosponge Beta, which is however prepared using complex and expensive multi-quaternary ammonium surfactants. Moreover, this synthetic protocol for 4-aryltetrahydropyrans replaces the carcinogenic and toxic chemicals, which have been previously used for Prins–Friedel–Crafts reactions, with green and non-toxic substances.
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- 2020
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4. Mordenite nanorods and nanosheets prepared in presence of gemini type surfactants
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Xiaodong Zou, Jiří Čejka, K. M. Konysheva, Mariya Shamzhy, Changhong Xiao, Maksym Opanasenko, Oleksiy V. Shvets, and Pavel S. Yaremov
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Materials science ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Catalysis ,Mordenite ,Nanocrystalline material ,0104 chemical sciences ,Microcrystalline ,Nanocrystal ,Chemical engineering ,Nanorod ,0210 nano-technology ,Selectivity ,Zeolite - Abstract
The influence of synthesis parameters (e.g. Si/Al ratio, pH of the reaction mixture, structure of Gemini-type surfactant) on the phase selectivity of nanocrystalline MOR formation was studied. The nature of organic structure-directing cation (i.e. charge, size) was found as a decisive factor controlling morphology of MOR nanocrystals. Fabricated nanocrystalline MOR zeolites showed enhanced textural characteristics (BET area, total pore volume) and higher catalytic activity (TOF = 42–45 vs. 15 h−1) in acid-catalyzed annulation reaction of 2-naphtol with methylbut-3-en-2-ol when compared to commercial microcrystalline MOR zeolite.
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- 2019
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5. Molecular insight on unusually high specific hydrogen adsorption over silicon carbide
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Atte Aho, Nataliya D. Shcherban, Pavel S. Yaremov, and Dmitry Yu. Murzin
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Materials science ,Renewable Energy, Sustainability and the Environment ,Energy Engineering and Power Technology ,chemistry.chemical_element ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,01 natural sciences ,Supercritical fluid ,Hydrogen adsorption ,0104 chemical sciences ,Carbide ,chemistry.chemical_compound ,Fuel Technology ,Adsorption ,chemistry ,Chemical engineering ,Silicon carbide ,Graphite ,0210 nano-technology ,Carbon ,Template method pattern - Abstract
Hydrogen adsorption over silicon carbide of different nature was investigated. High specific hydrogen adsorption (up to 15 μmol/m2), nontypical for silicon carbide was obtained for the materials prepared by the template method. A more perfect truly "carbide" structure (with a higher content of Si–C bonds in the form of carbide) in this type of materials contributes to an increase of the specific hydrogen adsorption. However, some non-stoichiometricity manifested in the presence of carbon in other (non-carbide) bonds (graphite or terminal and sp3 hybridized C) is required for exceptionally high specific hydrogen adsorption. The influence of the adsorbate nature for several gases (Н2, N2, CO) was found to be less prominent for SiC compared to carbon and silica materials. This feature inherent only to silicon carbide exhibiting an increased level of specific hydrogen adsorption, is due to cooperative adsorption, accompanied by an abnormally high loading of the adsorbent surface in the supercritical region.
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- 2019
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6. Hierarchical Beta zeolites obtained in concentrated reaction mixtures as catalysts in tetrahydropyranylation of alcohols
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Nataliya D. Shcherban, Roman Barakov, Pavel S. Yaremov, V. V. Tsyrina, Maksym Opanasenko, Igor Bezverkhyy, Laboratoire Interdisciplinaire Carnot de Bourgogne [Dijon] (LICB), and Université de Bourgogne (UB)-Université de Technologie de Belfort-Montbeliard (UTBM)-Centre National de la Recherche Scientifique (CNRS)
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010405 organic chemistry ,Process Chemistry and Technology ,Nanoparticle ,010402 general chemistry ,01 natural sciences ,Micelle ,Catalysis ,0104 chemical sciences ,law.invention ,Amorphous solid ,[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry ,chemistry.chemical_compound ,Chemical engineering ,chemistry ,law ,Aluminosilicate ,Bromide ,Crystallization ,Zeolite ,ComputingMilieux_MISCELLANEOUS - Abstract
Hierarchical zeolites consisting of Beta nanoparticles (15–40 nm) were obtained via hydrothermal treatment of a concentrated zeolite gel-precursor (H2O/Si = 2.5–14) without utilization of complex SDAs. The proposed approach is based on the formation of a large number of zeolite nuclei under particular crystallization conditions, followed by their agglomeration resulting in the dense packing of the particles preventing their further growth. The micelles of cetyltrimethylammonium bromide (CTAB) can be used to additionally limit the growth of zeolite nanoparticles during hydrothermal treatment of concentrated reaction mixtures. Such deceleration of crystallization promotes the formation of highly porous X-ray amorphous nanosized aluminosilicate. Due to the developed mesoporosity and increased accessibility to the acid sites for the molecules of a large size, hierarchical Beta zeolites obtained in the presence of CTAB demonstrate high catalytic activity in the reaction of bulky alcohols (1-octadecanol and 1-adamantanemethanol) with 3,4-dihydro-2H-pyran.
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- 2020
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7. Morphological features of porous silicon carbide obtained via a carbothermal method
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Svitlana Filonenko, Sergii A. Sergiienko, Nataliya D. Shcherban, M.A. Skoryk, Pavel S. Yaremov, Dmitry Yu. Murzin, and V. G. Ilyin
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Marketing ,Materials science ,Silicon ,chemistry.chemical_element ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,Porous silicon ,01 natural sciences ,0104 chemical sciences ,chemistry.chemical_compound ,chemistry ,Carbothermic reaction ,Materials Chemistry ,Ceramics and Composites ,Silicon carbide ,Fiber ,Composite material ,0210 nano-technology ,Porosity ,Mesoporous material ,Carbon - Abstract
Samples of porous silicon carbide were obtained using sucrose or carbon and aerosil or silica mesoporous molecular sieves (SBA-3, SBA-15, KIT-6 and MCF). Fibers content in silicon carbide samples is higher when the mesopore surface area of carbon materials derived from carbon-silica composites is lower. Based on the found correlation between the morphology and porosity of SiC and mesopore surface area of the carbon component in the composites, a templating action of carbon in carbothermal reduction was suggested.
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- 2017
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8. Influence of SBA-15 Zeolitization Conditions on Structural-Sorption and Acidic Properties of Micro-Mesoporous AluminosilicateS SBA-15/ZSM-5
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Pavel S. Yaremov, Svitlana Filonenko, Nataliya D. Shcherban, V. G. Ilyin, V. V. Tsyrina, and Roman Barakov
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Inorganic chemistry ,Sorption ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,chemistry.chemical_compound ,chemistry ,Aluminosilicate ,Hydroxide ,Lewis acids and bases ,Crystallite ,ZSM-5 ,0210 nano-technology ,Mesoporous material ,Brønsted–Lowry acid–base theory - Abstract
Partly zeolitized micro-mesoporous aluminosilicates SBA-15/ZSM-5 were synthesized by conversion of dry gel of template-containing SBA-15 in the presence of tetrapropylammonium hydroxide. They have a hexagonally ordered mesostructure and developed surface and mesoporosity for which the concentration and strength of the Bronsted and Lewis acid sites are higher than in AlSi-SBA-15. The formation of Bronsted acid sites of moderate strength in the samples with a low degree of zeolitization is due to the presence of ZSM-5 precursors as well as crystallites in the obtained aluminosilicates.
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- 2017
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9. Porosity Enhancement of Silicon Carbide by Preparation in Micro-Mesoporous Zeolite-Like Matrices
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Nataliya D. Shcherban, Svitlana Filonenko, and Pavel S. Yaremov
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Chemistry ,Inorganic chemistry ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Carbide ,chemistry.chemical_compound ,Adsorption ,Volume (thermodynamics) ,Chemical engineering ,Carbothermic reaction ,Silicon carbide ,0210 nano-technology ,Mesoporous material ,Zeolite ,Porosity - Abstract
Heat treatment of carbon–silica composites derived from micro-mesoporous zeolite-like materials yields the β-modification of silicon carbide with adsorption characteristics much superior to those of analogs obtained using large-porous silica exotemplates (meso-cellular foams). The presence of a large volume of relatively homogeneous mesopores, which permits us to achieve a close-to-stoichiometric C/SiO2 ratio, accounts for the formation of silica carbide with well-developed porosity.
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- 2017
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10. Synthesis of micro-mesoporous aluminosilicates on the basis of ZSM-5 zeolite using dual-functional templates at presence of micellar and molecular templates
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Igor Bezverkhyy, Nataliya D. Shcherban, Alexander E. Baranchikov, Vladimir G. Ilyin, Pavel S. Yaremov, V. V. Tsyrina, Vladimir V. Trachevskii, and Roman Barakov
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Chemistry ,Inorganic chemistry ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,01 natural sciences ,0104 chemical sciences ,law.invention ,chemistry.chemical_compound ,Mechanics of Materials ,law ,Aluminosilicate ,Specific surface area ,Critical micelle concentration ,Hydroxide ,General Materials Science ,Calcination ,Lamellar structure ,0210 nano-technology ,Zeolite ,Mesoporous material - Abstract
Micro-mesoporous aluminosilicates consisting of agglomerates of the ZSM-5 nanoparticles were obtained using dual-functional templates [C6H13–N+(CH3)2–C6H12–N+(CH3)2–C6H13](Br−)2 (C6–6–6Br2), [C8H17–N+(CH3)2–C6H12–N+(CH3)2–C8H17](Br−)2 (C8–6–8Br2). Aluminosilicates with randomly oriented flake-like particles built from ZSM-5 layers were obtained using [C16H33–N+(CH3)2–C6H12–N+(CH3)2–C6H13](Br−)2 (C16–6–6Br2). Use of С8–6–8Br2 and additive of cetyltrimethylammonium bromide CTAB (CTAB concentration is lower than the first critical micelle concentration, CMC1) leads to an increase of the total specific surface area, mesopore surface area and the mesopore size uniformity in the product, as well as the concentration of Bronsted acid sites accessible for bulk molecules. It is assumed that CTAB role is to limit the zeolite crystals growth. Addition of CTAB to С16–6–6Br2 (CTAB concentration is also lower than CMC1) promotes the formation of micro-mesoporous aluminosilicate possessing disordered lamellar mesostructure stable upon calcination which is characterized by a higher total specific surface area and better mesopores uniformity than ZSM-5 obtained in the presence of С16–6–6Br2. The additive of a molecular template tetrapropylammonium hydroxide (TPAOH) shifts the structure formation toward zeolite and leads to an increase in the ratio of concentrations of Bronsted and Lewis acid sites for the obtained aluminosilicates. The addition of small amounts of TPAOH into the reaction mixture (TPAOH/C16–6–6Br2 = 6.5·10−3) leads to formation of self-pillared aluminosilicate. In this material the nanoparticles act as “pillars” between the layers of ZSM-5 and thus contribute to retention of low-ordered lamellar mesostructure after calcination, leading to increase of the total specific surface area and improving mesopores uniformity.
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- 2017
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11. Carbothermal synthesis of porous silicon carbide using mesoporous silicas
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Nataliya D. Shcherban, V. G. Ilyin, Sergii A. Sergiienko, Dmitry Yu. Murzin, Pavel S. Yaremov, and Svitlana Filonenko
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Materials science ,Hydrogen ,Silicon ,Mechanical Engineering ,Inorganic chemistry ,chemistry.chemical_element ,Sorption ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Molecular sieve ,01 natural sciences ,0104 chemical sciences ,Crystal ,chemistry.chemical_compound ,chemistry ,Chemical engineering ,Mechanics of Materials ,Silicon carbide ,General Materials Science ,0210 nano-technology ,Mesoporous material ,Carbon - Abstract
Samples of crystal modifications of porous silicon carbide were obtained by carbothermal method using carbon precursors (sucrose, carbon) and aerosil or mesoporous silicas molecular sieves SBA-3, SBA-15, KIT-6, and MCF as silicon sources. Porous β-SiC samples obtained from carbon–silica composites are characterized by high structural and sorption characteristics (S BET up to 410 m2/g, V pore up to 1.0 cm3/g). High hydrogen adsorption capacity of silicon carbide samples based on KIT-6 (up to 1.24 wt% at 77 K and 1 atm.), considering low adsorption energy ( $$ \left| {\Delta \mu_{0} } \right|_{{{\text{H}}_{2} }} $$ ) up to 2.3 kJ/mol for SiC vs. ca. 5.0 kJ/mol for carbon), was determined. The highest ever reported value among the existing porous materials was observed for specific adsorption of H2 by SiC (specific adsorption on the pore surface, ρ up to 15 μmol/m2) corresponding to almost complete filling of the surface with hydrogen in the examined conditions (77 K, 1 atm.).
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- 2016
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12. Boron-doped nanoporous carbons as promising materials for supercapacitors and hydrogen storage
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Vladimir G. Ilyin, Vyacheslav S. Dyadyun, Nataliya D. Shcherban, Pavel S. Yaremov, Igor Bezverkhyy, and Svitlana Filonenko
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Materials science ,Nanoporous ,Mechanical Engineering ,Nanotechnology ,Sulfuric acid ,02 engineering and technology ,Microporous material ,Electrolyte ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Boric acid ,chemistry.chemical_compound ,Hydrogen storage ,chemistry ,Chemical engineering ,Mechanics of Materials ,General Materials Science ,0210 nano-technology ,Mesoporous material ,Porosity - Abstract
Boron-doped carbon nanostructures were obtained via template and bulk synthesis from sucrose in the presence of boric acid. Synthesized B-containing mesoporous materials are characterized by high spatial ordering, developed surface (up to 870 m2/g), and porosity (up to 1.2 cm3/g). The obtained B-doped microporous materials exhibit high interfacial capacitance (up to 0.36 F/m2), which is higher than the available literature data and enables the use of synthesized samples as materials of supercapacitors. The capacity of electric double layer up to 300 F/g using sulfuric acid as the electrolyte was accumulated on microporous B-doped carbons.
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- 2016
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13. Effect of the Structure and Acidity of Micro-Mesoporous Alumosilicates on Their Catalytic Activity in Cumene Cracking
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V. V. Tsyrina, Nataliya D. Shcherban, Yu. G. Voloshyna, V. G. Ilyin, Pavel S. Yaremov, R. Yu. Barakov, and M. M. Krylova
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Cumene ,Inorganic chemistry ,02 engineering and technology ,General Chemistry ,Microporous material ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Catalysis ,Template reaction ,chemistry.chemical_compound ,chemistry ,0210 nano-technology ,Zeolite ,Mesoporous material ,Benzene ,Selectivity - Abstract
Micro-mesoporous alumosilicates derived from zeolite ZSM-5 were obtained in dual template reaction media and in the presence of dual functional templates. It was shown that aluminosilicates with 0.15-0.25 zeolitization exhibit high catalytic activity in cumene cracking, approaching the activity of ZSM-5 and superior to ZSM-5 in total selectivity relative to the major products (propylene and benzene). Greater oligomerization of propylene is observed with increasing micropore volume and concentration of strong acid sites in the alumosilicates along with increased cumene conversion.
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- 2016
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14. Two-stage dual template alkali metal-free synthesis of micro-mesoporous aluminosilicates based on ZSM-5 zeolite precursors
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Nataliya D. Shcherban, Roman Barakov, Vladimir G. Ilyin, Pavel S. Yaremov, and Vladimir Solomakha
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Cumene ,Materials science ,Mechanical Engineering ,Inorganic chemistry ,Sorption ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Molecular sieve ,01 natural sciences ,0104 chemical sciences ,Catalysis ,chemistry.chemical_compound ,chemistry ,Mechanics of Materials ,Aluminosilicate ,General Materials Science ,Lewis acids and bases ,0210 nano-technology ,Zeolite ,Mesoporous material - Abstract
Carrying out the dual template synthesis (in the presence of molecular and micellar templates) in the alkali metal-free reaction media (pH 11.7–12) at a relatively low-temperature hydrothermal treatment (100–120 °C, duration 3–5 days) allowed to obtain micro-mesoporous aluminosilicates combining the properties of zeolite ZSM-5 and mesoporous molecular sieve AlSi-MCM-41. X-ray amorphous sol-precursors of ZSM-5 zeolite obtained by preliminary hydrothermal treatment of alkali metal-free reaction mixture at 160 °C and containing secondary building units of zeolite were used as initial substances for synthesis of micro-mesoporous aluminosilicates. During the joint formation of the structure of zeolite and mesoporous molecular sieve in one reaction mixture and in contiguous conditions close to optimal for their individual formation, composites zeolite/mesoporous molecular sieve were formed. The structural and sorption characteristics and acidity of the obtained composites differ from mechanical mixture of two phases. X-ray amorphous micro-mesoporous aluminosilicate with secondary building units and precursors of ZSM-5 in mesostructure is characterized by higher concentration and strength of Bronsted and Lewis acid sites as well as a higher catalytic activity in the reaction of cracking of cumene compared to AlSi-MCM-41 of similar composition. This aluminosilicate also exhibits a higher total selectivity toward the major products of reaction, in comparison with ZSM-5.
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- 2016
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15. Synthesis, structure and adsorption properties of nonstoichiometric carbon nitride in comparison with nitrogen-containing carbons
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Nataliya D. Shcherban, Vladimir G. Ilyin, Atte Aho, Svitlana Filonenko, M.A. Skoryk, Dmitry Yu. Murzin, and Pavel S. Yaremov
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Carbonization ,General Chemical Engineering ,Inorganic chemistry ,chemistry.chemical_element ,02 engineering and technology ,Nitride ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Molecular sieve ,01 natural sciences ,Nitrogen ,0104 chemical sciences ,chemistry.chemical_compound ,Adsorption ,chemistry ,Specific surface area ,0210 nano-technology ,Carbon ,Carbon nitride - Abstract
The samples of nonstoichiometric carbon nitride characterized by spatial ordering, large pore volume (up to 0.8 cm3/g) and specific surface area (up to 585 m2/g) were obtained via matrix carbonization of ethylenediamine in the presence of carbon tetrachloride in mesoporous molecular sieves KIT-6 and MCF as exotemplates. In contrast to nitrogen-containing carbons (obtained by modification of carbon samples with nitrogen in the result of compatible thermal treatment of the initial porous carbon with melamine) nonstoichiometric carbon nitride contains much more nitrogen (up to 13.7 wt.% (C/N = 6), compared with preceding 0.6 wt.%) and increased the quantity of basic nitrogen-containing groups (in particular, amino groups)—up to 0.68 mmol/g (vs. 0.46 mmol/g). The increase of adsorption capacity towards hydrogen and carbon dioxide: adsorption potential, differential heat of CO2 adsorption, specific adsorption on the pore surface—from 5.4 to 7.3 μmol H2/m2 and from 2.2 to 5.4 μmol CO2/m2 for carbon and synthesized samples of nonstoichiometric carbon nitride, respectively, due to the incorporation of nitrogen atoms into the carbon framework was noticed.
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- 2016
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16. Low-temperature and alkali-free dual template synthesis of micro-mesoporous aluminosilicates based on precursors of zeolite ZSM-5
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Nataliya D. Shcherban, Vladimir G. Ilyin, Pavel S. Yaremov, Roman Barakov, Nataliia Kasian, Svitlana Gryn, Vladimir Solomakha, and Igor Bezverkhyy
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Materials science ,Mechanical Engineering ,Inorganic chemistry ,Sorption ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Molecular sieve ,01 natural sciences ,0104 chemical sciences ,Adsorption ,Mechanics of Materials ,Aluminosilicate ,Desorption ,General Materials Science ,ZSM-5 ,0210 nano-technology ,Zeolite ,Mesoporous material - Abstract
The aim of this study was to determine the influence of the conditions of low-temperature sequential dual template synthesis of micro-mesoporous aluminosilicates based on precursors of ZSM-5 on their phase composition, structure, sorption properties, and acidity. The methods of X-ray powder diffraction and volumetric adsorption (N2, 77 K) analysis, dynamic light scattering (for characterization of sol-precursors), IR-spectroscopy, energy-dispersive X-ray spectroscopy, scanning and transmission electron microscopy, solid-state 29Si MAS NMR and 29Si{1H} cross-polarization MAS NMR spectroscopy, temperature-programmed desorption of ammonia, ad(de)sorption of pyridine and 2,6-di-tert-butylpyridine with IR-spectral control were used for characterization of the obtained micro-mesoporous aluminosilicates. It was shown that the convergence of compositions of the reaction mixtures and conditions of formation of zeolites and mesoporous molecular sieves, in particular, the use of alkali-free reaction medium and relatively low temperature of hydrothermal treatment (100 °C) allowed to obtain the X-ray amorphous and partially zeolitized micro-mesoporous aluminosilicates. Such aluminosilicates have appropriate structural and sorption properties and the acidity inherent to ZSM-5 and MCM-41, including the Bronsted and Lewis acid sites which are accessible for bulk molecules of organic substances. The possibility of purposeful regulation of characteristics of micro-mesoporous aluminosilicates depending on the conditions of their preparation was confirmed. Herewith the investigated aluminosilicates possess the sorption and acidic properties which are different from the mechanical mixture of two phases.
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- 2016
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17. Low-temperature synthesis, structure, sorption properties and acidity of zeolite ZSM-5
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Vladimir G. Ilyin, Roman Barakov, Vladimir Solomakha, Nataliya D. Shcherban, Pavel S. Yaremov, and Aleksey Vyshnevskyy
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Cumene ,Mechanical Engineering ,Inorganic chemistry ,Sorption ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Catalysis ,Styrene ,chemistry.chemical_compound ,chemistry ,Mechanics of Materials ,Specific surface area ,Organic chemistry ,General Materials Science ,ZSM-5 ,0210 nano-technology ,Zeolite ,Selectivity - Abstract
High structure-directing activity and specificity of templating action of tetrapropylammonium cations TPA+ as well as high concentration of framework-forming substances in the initial reaction mixtures contribute to the formation of zeolite ZSM-5 at relatively low temperature (100 °C) in the alkali-free media. Zeolite ZSM-5 obtained at 100 °C has higher micropore and mesopore volumes, specific surface area, less uniform micropore size distribution in comparison with ZSM-5 synthesized at 170 °C in an alkaline medium in the presence of hydrated Na+ cations. Samples synthesized at 100 °C possess a lower concentration of acid sites and broader distribution of them in strength, compared with ZSM-5 obtained at 170 °C in an alkaline medium. ZSM-5 obtained at 100 °C exhibits a high catalytic activity in the reaction of cracking of cumene, as well as a higher selectivity to propylene and styrene, in comparison with isostructural analogue obtained at 170 °C in an alkaline medium. It is assumed that the investigated alkali-free reaction mixtures and the corresponding sol-precursors of zeolite ZSM-5 containing the elements of secondary building units can be used for obtaining of micro-mesoporous aluminosilicates in the conditions of low-temperature synthesis (100 °C) by dual-template method—in the presence of molecular and micellar templates.
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- 2015
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18. Structure and Porosity of Silicon Carbide Produced by Matrix Method
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Nataliya D. Shcherban, Svitlana Filonenko, Sergii A. Sergiienko, V. G. Ilyin, and Pavel S. Yaremov
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Matrix (chemical analysis) ,chemistry.chemical_compound ,chemistry ,Chemical engineering ,Carbothermic reaction ,Silicon carbide ,chemistry.chemical_element ,General Chemistry ,Molecular sieve ,Mesoporous material ,Porosity ,Carbon ,Stoichiometry - Abstract
Silicon carbide in the $$ \beta $$ modification with a developed surface and a large pore size was obtained by carbothermal reduction using mesoporous siliceous molecular sieves (SBA-15, KIT-6, MCF, SBA-3). The formation of silicon carbide with high porosity parameters is favored by the use of the KIT-6 mesoporous molecular sieve (MMS) with a three-dimensional structure and a mutually intersecting system of mesopores as matrix, by the close to the stoichiometric C/SiO2 ratio, and also by the higher level of filling with carbon in the pores of the siliceous MMS.
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- 2015
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19. Influence of thermal treatments on phase composition and acidity of mesoporous tungsten oxide
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Nataliia Kasian, Pavel S. Yaremov, Eric Puzenat, Alain Tuel, Oleksiy V. Shvets, Laurence Burel, MATERIAUX (MATERIAUX), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), +LBU, and AIR:EAU+EPU
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Materials science ,Inorganic chemistry ,chemistry.chemical_element ,[CHIM.CATA]Chemical Sciences/Catalysis ,General Chemistry ,Tungsten ,Silicotungstic acid ,Condensed Matter Physics ,[SDE.ES]Environmental Sciences/Environmental and Society ,law.invention ,chemistry.chemical_compound ,Adsorption ,chemistry ,Mechanics of Materials ,law ,Chemisorption ,General Materials Science ,Calcination ,Orthorhombic crystal system ,Mesoporous material ,Monoclinic crystal system - Abstract
AIR:EAU:MATERIAUX+NKS:LBU:EPU:ATU; We report on the synthesis of mesoporous tungsten oxides via hard templating method using silicotungstic acid as W precursor and having surface areas and pore diameters up to 68 m(2)/g and 12.8 nm, respectively. The relation between thermal treatments (calcination temperature of W-KIT-6 composites and reductive treatment of tungsten oxides), crystalline structure and acidity has been systematically investigated. The acidity of mesoporous tungsten oxides was investigated using common pyridine adsorption methods and chemisorption of probe molecules (CO, H-2). Combination of XRD and FTIR techniques showed that monoclinic and orthorhombic phases of crystalline wall structure coexist in the calcination temperatures 550-800 degrees C. Increasing the calcination temperature and decreasing the W/Si mass ratio of composites favors the transformation of orthorhombic phase to more stable monoclinic. Moreover, the acidity as well as ability to chemisorbs CO decreases when the calcination temperature increases. The concentration of acid sites also depends on the temperature of reductive treatment of tungsten oxides: CO uptakes increase twice at the 250 degrees C and decrease by four times when the temperature increases to 450 degrees C. (C) 2014 Elsevier Inc. All rights reserved.
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- 2014
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20. Influence of the method of activation on the structural and sorption properties of the products of carbonization of sucrose
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Pavel S. Yaremov, Vladimir G. Ilyin, Mariya V. Ovcharova, and Nataliya D. Shcherban
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Carbonization ,Chemistry ,Inorganic chemistry ,Sorption ,Microporous material ,Analytical Chemistry ,Catalysis ,chemistry.chemical_compound ,Fuel Technology ,Adsorption ,Chemical engineering ,Specific surface area ,Mesoporous material ,Phosphoric acid - Abstract
The comparative research of bulk carbonization of sucrose at different temperatures (Ar, 400–900 °C) in the presence of activating agents (H 3 PO 4 and ZnCl 2 ) and water vapor was carried out. X-ray diffraction, nitrogen and hydrogen adsorption and IR spectroscopy were used for investigating of the structural and sorption characteristics of the obtained materials. It was shown that in conditions of non-catalytic bulk carbonization of sucrose homogeneous microporous carbons were formed; with the increasing of the temperature of carbonization micropore volume and adsorption of hydrogen (up to 1.48 wt.%, 900 °C) were increased. The essential effect of using an activating agent and/or catalytic agent on the porous structure of carbons: in the presence of phosphoric acid carbons with increased micro- and supermicropore volume were obtained. Mainly mesoporous carbons were formed in the presence of zinc chloride. It was established that thermal activation with steam at 800 and 850 °C results in the significant increase of specific surface area of the carbons ( S BET – up to 2287 m 2 /g) and hydrogen adsorption – up to 1.88 and 1.99 wt.% accordingly.
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- 2014
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21. Synthesis and physical–chemical properties of N-containing nanoporous carbons
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Nataliya D. Shcherban, Pavel S. Yaremov, Vyacheslav S. Dyadyun, and Svitlana Filonenko
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Materials science ,Nanoporous ,Carbonization ,Mechanical Engineering ,Inorganic chemistry ,chemistry.chemical_element ,Microporous material ,Nitrogen ,Matrix (chemical analysis) ,chemistry.chemical_compound ,Adsorption ,chemistry ,Chemical engineering ,Mechanics of Materials ,Urea ,General Materials Science ,Melamine - Abstract
Meso- and microporous nitrogen-containing carbons, characterized by homogeneous meso- (V = 1.00 cm3/g, D = 3.5 nm) and microporous (V up to 0.26 cm3/g, D ≈ 0.5 nm) structure, and the presence of basic groups (up to 1.7 mmol/g) were obtained by matrix and bulk carbonization of sucrose in the presence of melamine or urea. It is shown that obtained N-containing microporous carbons possess good interfacial capacitance (0.21 F/m2) and they are characterized with stability during repeated charge–discharge cycles. Synthesized N-containing nanoporous carbons show higher adsorption of carbon dioxide (up to 6.3 mmol/g at −20 °C) than the samples without nitrogen (up to 3.9 mmol/g at −20 °C).
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- 2014
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22. Template synthesis, structure, sorption properties and acidity of micro-mesoporous materials obtained from sol-precursor of zeolite BEA
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Vladimir Solomakha, Pavel S. Yaremov, Nataliya D. Shcherban, Vladimir G. Ilyin, Svitlana Gryn, Roman Barakov, and Olena Khaynakova
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Materials science ,Mechanical Engineering ,Sorption ,Microporous material ,Molecular sieve ,Amorphous solid ,law.invention ,Chemical engineering ,Mechanics of Materials ,law ,Specific surface area ,Organic chemistry ,General Materials Science ,Crystallization ,Mesoporous material ,Zeolite - Abstract
Partially zeolitized micro-mesoporous materials (the total specific surface area S BET = 460–645 m2/g, mesopore volume V meso = 0.30–0.57 cm3/g, mesopore diameter D meso ≈ 5.6 nm, micropore volume V micro = 0.11–0.16 cm3/g, micropore diameter D micro ≈ 0.72 nm) and X-ray amorphous micro-mesoporous materials with uniform mesoporous structure (mesopore specific surface area S meso = 820–890 m2/g, total pore volume V t = 0.71–0.86 cm3/g, V meso = 0.53–0.67 cm3/g, D meso = 1.8–2.4 nm) were obtained by micellar templating of sol-precursor containing primary products of crystallization of zeolite BEA under conditions typical for forming of mesoporous molecular sieve MCM-41 (hydrothermal treatment at 100–130 °C for 3–5 days). It was found that the obtained X-ray amorphous micro-mesoporous materials contain secondary building units of zeolite BEA (five-membered rings of Si–O tetrahedra of BEA) and show acidic properties comparable to zeolite BEA.
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- 2014
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23. Effect of Dual Template Synthesis Conditions on Structural/Sorption Properties and Acidity of Microporous/Mesoporous ZSM-5/MCM-41 Aluminosilicates
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Vladimir Solomakha, Svitlana Gryn, Nataliya D. Shcherban, Vladimir G. Ilyin, Pavel S. Yaremov, R. Yu. Barakov, and Olena Khaynakova
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MCM-41 ,Chemistry ,Aluminosilicate ,Inorganic chemistry ,Sorption ,General Chemistry ,Microporous material ,ZSM-5 ,Zeolite ,Mesoporous material ,Amorphous solid - Abstract
We have used a dual template synthesis method based on an initial ZSM-5 zeolite sol precursor in the presence of molecular and micellar templates to obtain X-ray amorphous and zeolite-containing microporous/mesoporous aluminosilicates having an ordered MCM-41 mesostructure, extended mesoporosity, small micropore volume, and medium-strength acid sites. We note a deviation from additivity for the change in micropore volume and the concentration of acid sites in the synthesized zeolitized samples.
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- 2013
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24. The influence of preparation conditions and doping on the physicochemical and sensor properties of mesoporous tin oxide
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Sergiy A. Sergiienko, Оlexander L. Kukla, Volodymyr N. Solomakha, Oleksiy V. Shvets, and Pavel S. Yaremov
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Materials science ,Thin layers ,Nanocomposite ,Tin dioxide ,Inorganic chemistry ,Metals and Alloys ,Sorption ,Condensed Matter Physics ,Tin oxide ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials ,Mesoporous organosilica ,chemistry.chemical_compound ,chemistry ,Materials Chemistry ,Thermal stability ,Electrical and Electronic Engineering ,Mesoporous material ,Instrumentation - Abstract
The influence of conditions used for preparation of mesoporous materials and thin layers based on tin oxide on physicochemical and sensor properties of these materials were studied. Thermal stability, acidic, sorption and electric properties were studied. The advantage of thin (≈1 μm) thermostable nanocomposite layers with relatively high parameters of the porous structure ( V = 0.460 cm 3 /g, S ВЕТ = 440 m 2 /g) was shown. Obtained materials can be used for selective gas/vapor sensing.
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- 2013
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25. Highly acidic phosphorus-containing porous carbons: synthesis and physicochemical properties
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Mariya V. Ovcharova, Vladimir G. Ilyin, Nataliya D. Lysenko, and Pavel S. Yaremov
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Aqueous solution ,Chemistry ,Mechanical Engineering ,Phosphorus ,Inorganic chemistry ,Potentiometric titration ,chemistry.chemical_element ,Sorption ,chemistry.chemical_compound ,Adsorption ,Mechanics of Materials ,General Materials Science ,Pyrolysis ,Carbon ,Phosphoric acid - Abstract
Phosphorus-containing carbon porous materials were obtained by pyrolysis of sucrose in the presence of phosphoric acid at a temperature 400 and 800 °C. Synthesized samples were characterized by elemental analysis, infrared spectroscopy, nitrogen adsorption–desorption, the measurement of cation-exchange capacity (CEC) and sorption capacity for lead ions, potentiometric titration. It was shown that phosphorus-containing carbon sorbents have acidic properties and they are characterized by high cation-exchange capacity (up to 5.9 mmol/g). The samples which were synthesized at 800 °C have the highest content of acid groups, as well as phosphorus and oxygen. Detected surface acidic groups are phosphorus-containing (pК ~1.7–1.9) and represent residua of acid phosphates and polyphosphates, connected with carbon framework. High CEC of synthesized materials can be attributed to a significant degree of phosphorylation of sucrose through the large number of hydroxyl groups. P-containing acid groups on the surface of carbon framework provide high adsorption of heavy metals ions (in particular lead). Thus, the obtained P-containing carbon sorbents can be used as effective cation-exchangers for the removal of cations of heavy metals from aqueous solutions.
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- 2011
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26. Conditions and features of matrix and bulk carbonization of the organic precursors
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Pavel S. Yaremov, Vladimir G. Ilyin, Mariya V. Ovcharova, and Nataliya D. Lysenko
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Materials science ,Carbonization ,Mechanical Engineering ,Inorganic chemistry ,chemistry.chemical_element ,Sorption ,Microporous material ,Adsorption ,chemistry ,Mechanics of Materials ,General Materials Science ,Graphite ,Mesoporous material ,Carbon ,Pyrolysis - Abstract
Comparative research of matrix and bulk carbonization of some organic precursors (sucrose, acetonitrile) in silica mesoporous materials SBA-15 and KIT-6 was conducted. X-ray diffraction, nitrogen adsorption analysis, Raman spectroscopy were used for determination of the structural-sorption characteristics of the obtained materials. It was shown that the carbon mesoporous materials CMK-8 obtained in the mesopores of KIT-6 had higher adsorption characteristics because of features of three-dimensional cubic structure, larger pore volume and framework’s wall thickness. It was established that partially graphitized spatially well-organized carbon materials were formed as a result of pyrolysis of acetonitrile in the silica matrices SBA-15 and KIT-6. It was conditioned by the absence of considerable spatial limitations for growth of graphite structures on the initial stage of the synthesis when the pores of the matrix were not filled up with the organic precursor. Product of bulk carbonization of sucrose is compact carbon microporous framework with low sorption characteristics (micropore volume is 0.09 cm3/g).
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- 2011
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27. Isomorphous Introduction of Boron in Germanosilicate Zeolites with UTL Topology
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Dana Procházková, Mariya Shamzhy, Oleksiy V. Shvets, Pavel S. Yaremov, Zuzana Musilová, and Jiří Čejka
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Chemistry ,General Chemical Engineering ,Inorganic chemistry ,chemistry.chemical_element ,General Chemistry ,Topology ,Adsorption ,Phase (matter) ,Materials Chemistry ,Selectivity ,Zeolite ,Boron ,Chemical composition ,Topology (chemistry) - Abstract
The direct introduction of boron into the framework of germanosilicate zeolites with UTL topology using different organic spiro azo compounds as structure-directing agents (SDAs) was performed. The influence of the SDA's nature, chemical composition and pH of the reaction mixture, and duration of the synthesis on the phase selectivity, limit of isomorphous introduction of boron into the zeolite framework and its location and coordination, and adsorption and acidic properties of prepared borogermanosilicates was investigated in detail. Experimental data provided clear evidence that the properties of the SDAs control the upper limit of the B content in the reaction mixture for successful synthesis of a pure UTL phase. UTL is formed in the pH region having the highest concentration of Ge8O15(OH)53– (D4R) in water. In synthesized UTL samples the contents of Si and Ge depend particularly on the pH values of the reaction mixtures with similar chemical compositions. With increasing pH of the reaction mixture, th...
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- 2011
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28. Structural and sorption properties of carbon replicas obtained by matrix carbonization of organic precursors in SBA-15 and KIT-6
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V. G. Il'in, Pavel S. Yaremov, Maksym Opanasenko, N. D. Lysenko, and A. V. Shvets
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chemistry.chemical_compound ,Adsorption ,chemistry ,Carbonization ,Specific surface area ,Inorganic chemistry ,Polyacrylonitrile ,chemistry.chemical_element ,Sorption ,General Chemistry ,Molecular sieve ,Mesoporous material ,Carbon - Abstract
We have carried out a comparative study of matrix carbonization of some organic precursors (sucrose, polydivinylbenzene, polyphenol-formaldehyde, polyacrylonitrile, acetonitrile) in SBA-15 and KIT-6 silica mesoporous molecular sieves. We have shown that carbon mesoporous molecular sieves of the CMK-8 type, obtained in KIT-6 mesopores, have better adsorption characteristics due to the features of the three-dimensional cubic structure, the larger pore volume and thickness of the walls of the framework. The maximum micropore volume is observed in CMK-3 and CMK-8, obtained by carbonization of polyphenol-formaldehyde and polydivinylbenzene, while the greatest specific surface area is observed on carbonization of sucrose, where the maximum hydrogen adsorption capacity is achieved at a level of ∼1.4 wt.% (77 K, 1 atm). We show that the mesopore surface coverage by hydrogen in carbon mesoporous molecular sieves increases as the degree of graphitization increases.
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- 2010
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29. The influence of metal nature on the structure, adsorption and acidic properties of aluminophosphate with VFI structure
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Oleksiy V. Shvets, Vladimir G. Ilyin, and Pavel S. Yaremov
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Metal ,Electronegativity ,Adsorption ,Ionic radius ,Chemistry ,visual_art ,Inorganic chemistry ,visual_art.visual_art_medium ,Zeolite ,Molecular sieve - Abstract
Metaloaluminophosphate zeolites with VFI structure, containing incorporated metals cations, were synthesized. Essential deformation of VFI structure, correlating with the size of ionic radii of incorporated cation is found. The formation of strong acid centers was detected in the case of bivalent cation and Cr 3+ . It was established, that the stregth of the Bronsted acidic centers is sharply reduced in a sequence of substitution cations Mg >> Ca > Sr≥ Ba and grows in a sequence Cu ≤ Ni≤ Mn≤ Co < Zn < Cr < Mg, which may evidence for cumulative influence of electronegativity and the radius of metals cation on value of Me-O(H)-P angle and strength of the acidic centers.
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- 2008
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30. Synthesis of isomorphously substituted extra-large pore UTL zeolites
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Jiří Čejka, Oleksiy V. Shvets, Liana G. Sarkisyan, Pavla Chlubná, Martin Hartmann, Arnošt Zukal, Mariya Shamzhy, Pavel S. Yaremov, V. R. Reddy Marthala, and Maksym Opanasenko
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Chemistry ,Heteroatom ,Substituent ,General Chemistry ,Large pore ,law.invention ,chemistry.chemical_compound ,law ,Phase (matter) ,Materials Chemistry ,Organic chemistry ,Physical chemistry ,Composition (visual arts) ,Crystallization ,Selectivity ,Zeolite - Abstract
The influence of various synthesis parameters (e.g. gel composition, pH of the reaction mixture, duration of crystallization) on the phase selectivity of zeolite formation in germanosilicate reaction medium in the presence of different three-valent heteroatoms (B, Al, Ga, Fe or In) was systematically studied and compared with a controlled crystallization from pure germanosilicate media. The boundary conditions of the formation of the pure phase of isomorphously substituted extra-large pore zeolite UTL were established. In the presence of 1 mol% of the respective heteroelement in the initial gel the pH borders of UTL formation are found to be 7.5–11.9 for Fe-, 7.8–12.0 for B-, 8.2–11.0 for Ga-, 11.0–12.0 for In-, and 11.3–12.0 for Al-containing reaction mixtures. The maximum concentration of heteroelements in the reaction mixture for the successful synthesis of UTL is 1.5 mol% for Al and Ga, 6 mol% for In, and 13 mol% for B. The size of UTL crystals decreases in the order Al- > In- > Ga- > Fe- ≈ B-UTL. The nature of isomorphous substituent influences the textural properties (pore size distribution) of the respective UTL zeolites.
- Published
- 2012
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Catalog
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