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Ab-initio study of hydrogen chemical adsorption on the platinum surface/carbon nanotube join system [Text] / A. S. Fedorov, P. B. Sorokin, A. A. Kuzubov // Physica status solidi B - Basic Solid State Physics. - 2008. - Vol. 245, № 8. - P1546-1551

Доп.точки доступа:
Fedorov, A.S.; Sorokin, P.B.; Kuzubov, A. A.
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Adsorption of organic dyes by Fe3O4@C, Fe3O4@C@C, and Fe3O4@SiO2 magnetic nanoparticles / O. S. Ivanova, I. S. Edelman, A. E. Sokolov [et al.] // Bull. Russ. Acad. Sci. Phys. - 2023. - Vol. 87, Is. 3. - P. 338-342, DOI 10.3103/S1062873822701192. - Cited References: 17. - This research was funded partly by the Ministry of Science and Higher Education of the Russian Federation, project FWES-2021-0035. Ch. R. Lin and Yu. Zh. Chen thank the National Science and Technology Council of Taiwan for the financial support, MOST no. 110-2112-M-153-005- and no. 108-2923-M-153-001-MY3 . - ISSN 1062-8738. - ISSN 1934-9432
Аннотация: Fe3O4@C, Fe3O4@C@C, and Fe3O4@SiO2 core–shell nanoparticles are synthesized via thermal decomposition and coprecipitation. Samples are characterized via X-ray spectroscopy, transmission electron microscopy, and magnetometry. It is shown that the magnetic core of all nanoparticles is nanocrystalline and has crystal parameters corresponding to only one phase of Fe3O4, covered with a uniform shell of amorphous carbon or silicon oxide around 8 nm thick. Special attention is given to adsorption properties of the nanoparticles with respect to four dyes: Methylene blue, Congo Red, Eosin Y, and Rhodamine C. The high selectivity of Fe3O4@C nanoparticles to various dyes is revealed.

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Публикация на русском языке Адсорбция органических красителей магнитными наночастицами Fe3O4@C, Fe3O4@C@C, Fe3O4@SiO2 [Текст] / О. С. Иванова, И. С. Эдельман, А. Э. Соколов [и др.] // Изв. РАН. Сер. физич. - 2023. - Т. 87 № 3. - С. 390-395

Держатели документа:
Kirensky Institute of Physics, Siberian Branch, Russian Academy of Sciences, 660036, Krasnoyarsk, Russia
Siberian Federal University, 660041, Krasnoyarsk, Russia
National Pingtung University, 900392, Pingtung, Taiwan

Доп.точки доступа:
Ivanova, O. S.; Иванова, Оксана Станиславовна; Edelman, I. S.; Эдельман, Ирина Самсоновна; Sokolov, A. Е.; Соколов, Алексей Эдуардович; Svetlitsky, E. S.; Светлицкий, Евгений Сергеевич; Zharkov, S. M.; Жарков, Сергей Михайлович; Sukhachev, A. L.; Сухачев, Александр Леонидович; Lin, Ch. R.; Chen, Yu. Zh.
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Adsorption properties and catalytic activity of Fe3O4-Ag nanostructures / O. S. Ivanova, Ch.-R. Lin, I. S. Edelman [et al.] // Appl. Surf. Sci. - 2024. - Vol. 665. - Ст. 160236, DOI 10.1016/j.apsusc.2024.160236. - Cited References: 48. - The work is supported by the Russian Science Foundation (project no. 23-22-10025, https://rscf.ru/project/ 23-22-10025/) and by the Krasnoyarsk Regional Fund of Science and Technology Support. The electron microscopy and EDS investigations were conducted in the SFU Joint Scientific Center. Magnetic investigations were carried out in the Krasnoyarsk Regional Center of Research Equipment of Federal Research Center "Krasnoyarsk Science Center SB RAS" . - ISSN 0169-4332. - ISSN 1873-5584
Кл.слова (ненормированные):
FeO-Ag nanostructures -- Nano-adsorbents -- Water purification methods -- Catalytic activity of nanoparticles
Аннотация: The morphology and magnetic properties as well as adsorption capacity and catalytic activity of Fe3O4-Ag nanoparticles synthesized by the solvothermal method were studied in dependence on the duration of the thermolysis process (3, 6, and 8 h). X-ray diffraction, transmission electron microscopy, and energy-dispersive spectroscopy measurements showed that the morphology of nanoparticles changed strongly as the duration of thermolysis increased. At 6 and 8 h duration, Fe3O4 nanocrystals grow and assemble into porous spherical globules with an Ag core (samples 2 and 3). These samples demonstrate high magnetization value and very low coercivity. The adsorption capacity of nanoparticles was studied with respect to two organic dyes: cationic methylene blue (MB) and anionic Congo red (CR). The particles showed preferential adsorption of the cationic dye. High catalytic activity towards four dyes: MB, methyl orange (MO), CR, and Rhodamine C (RhC) at the presence of NaBH4 is the remarkable property of these samples. The rate constant of the catalytic reaction was 1.4 min−1. Simultaneous exposure of CR and MO dyes to nanoparticles and NaBH4 caused their irreversible 100 % degradation while in the case of MB and RhC, a transition to their leuco form occurred.

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Держатели документа:
Kirensky Institute of Physics, Federal Research Center KSC Siberian Branch, Russian Academy of Sciences, Krasnoyarsk 660036, Russia
Siberian Federal University, Krasnoyarsk 660041, Russia
Department of Applied Physics, National Pingtung University, Pingtung City 90003, Taiwan
Institute of Chemistry and Chemical Technology, Federal Research Center KSC Siberian Branch, Russian Academy of Sciences, Krasnoyarsk 660036, Russia

Доп.точки доступа:
Ivanova, O. S.; Иванова, Оксана Станиславовна; Lin, Chun-Rong; Edelman, I. S.; Эдельман, Ирина Самсоновна; Svetlitsky, E. S.; Светлицкий, Евгений Сергеевич; Sokolov, A. Е.; Соколов, Алексей Эдуардович; Zharkov, S. M.; Жарков, Сергей Михайлович; Sukhachev, A. L.; Сухачев, Александр Леонидович; Vorobyev, S. A.; Petrov, D. A.; Петров, Дмитрий Анатольевич; Lin, En-Szu
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    Amino-functionalized Fe3O4@SiO2 core-shell magnetic nanoparticles for dye adsorption / C.-R. Lin, O. S. Ivanova, D. A. Petrov [et al.] // Nanomaterials. - 2021. - Vol. 11, Is. 9. - Ст. 2371, DOI 10.3390/nano11092371. - Cited References: 35. - The authors are thankful for the financial support the Russian Foundation for Basic Research, Grant № 19-52-52002, Ministry of Science and Technology of Taiwan, Grants MOST № 108-2923-M-153-001-MY3 and № 109-2112-M-153-003-, the Russian Foundation for Basic Research with Government of Krasnoyarsk Territory, Krasnoyarsk Regional Fund of Science, the research project number 19-42-240005: “Features of the electronic structure, magnetic properties and optical excitations in nanocrystals of the multifunctional magnetic chalcogenides Fe3S4 and FeSe”. We thank also the SFU Joint Scientific Center supported by the State assignment (#FSRZ-2020-0011) of the Ministry of Science and Higher Education of the Russian Federation, where the Transmission Electron Microscopy studies were carried out . - ISSN 2079-4991
   Перевод заглавия: Амино-функциональные магнитные наночастицы ядро-оболочка Fe3O4@SiO2 для адсорбции красителей
Кл.слова (ненормированные):
Fe3O4@SiO2 -- core-shell nanoparticles -- magnetic properties -- water pollutions -- fluorescence -- adsorption
Аннотация: Fe3O4@SiO2 core-shell nanoparticles (NPs) were synthesized with the co-precipitation method and functionalized with NH2 amino-groups. The nanoparticles were characterized by X-ray, FT-IR spectroscopy, transmission electron microscopy, selected area electron diffraction, and vibrating sample magnetometry. The magnetic core of all the nanoparticles was shown to be nanocrystalline with the crystal parameters corresponding only to the Fe3O4 phase covered with a homogeneous amorphous silica (SiO2) shell of about 6 nm in thickness. The FT-IR spectra confirmed the appearance of chemical bonds at amino functionalization. The magnetic measurements revealed unusually high saturation magnetization of the initial Fe3O4 nanoparticles, which was presumably associated with the deviations in the Fe ion distribution between the tetrahedral and octahedral positions in the nanocrystals as compared to the bulk stoichiometric magnetite. The fluorescent spectrum of eosin Y-doped NPs dispersed in water solution was obtained and a red shift and line broadening (in comparison with the dye molecules being free in water) were revealed and explained. Most attention was paid to the adsorption properties of the nanoparticles with respect to three dyes: methylene blue, Congo red, and eosin Y. The kinetic data showed that the adsorption processes were associated with the pseudo-second order mechanism for all three dyes. The equilibrium data were more compatible with the Langmuir isotherm and the maximum adsorption capacity was reached for Congo red.

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Держатели документа:
Department of Applied Physics, National Pingtung University, Pingtung City, 90003, Taiwan
Kirensky Institute of Physics, FRC KSC SB RAS, Krasnoyarsk, 660036, Russian Federation
Institute of Engineering Physics and Radio Electronics, Siberian Federal University, Krasnoyarsk, 660041, Russian Federation

Доп.точки доступа:
Lin, C. -R.; Ivanova, O. S.; Иванова, Оксана Станиславовна; Petrov, D. A.; Петров, Дмитрий Анатольевич; Sokolov, A. Е.; Соколов, Алексей Эдуардович; Chen, Y. -Z.; Gerasimova, M. A.; Zharkov, S. M.; Жарков, Сергей Михайлович; Tseng, Y. -T.; Shestakov, N. P.; Шестаков, Николай Петрович; Edelman, I. S.; Эдельман, Ирина Самсоновна
}
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Buckminsterfullerene's movability on the Fe(001) surface / A. A. Kuzubov [et al.] // J. Magn. Magn. Mater. - 2016. - Vol. 410. - P. 41-46, DOI 10.1016/j.jmmm.2016.03.023. - Cited References: 32. - This work was supported by the Russian Scientific Fund (Project no. 14-13-00139) and the Foundation for Assistance to Small Innovative Enterprises (FASIE) (Project no. 0011742). The authors would like to thank Institute of Computational Modeling of SB RAS, Krasnoyarsk; Joint Supercomputer Center of RAS, Moscow; Center of Equipment for Joint Use of Siberian Federal University, Krasnoyarsk; ICC of Novosibirsk State University and Siberian Supercomputer Center (SSCC) of SB RAS, Novosibirsk for providing the access to their supercomputers. . - ISSN 0304-8853

РУБ Materials Science, Multidisciplinary + Physics, Condensed Matter
Рубрики:
Initio molecular-dynamics
Total-energy calculations
Augmented-wave
Кл.слова (ненормированные):
Buckminsterfullerene -- C60 -- Fe(001) -- Spintronics -- Adsorption -- Relocation -- DFT
Аннотация: Organic-based spintronics is one of the most fast-developing fields in nanoelectronics. Buckminsterfullerene-based composites are widely investigated due to its unique properties and there is a number of studies concerned with its interfaces with various types of substrates. Ferromagnetic surfaces are of a particular interest for potential spintronics applications. Based on the data reported in literature, we suppose that there are more than one stable structure in C60/Fe(001) composite system. Here we investigate different possible adsorption sites of C60 molecule and reveal the possibility of their coexistence and its influence on the composite properties. © 2016 Elsevier B.V.

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Держатели документа:
Siberian Federal University, 79 Svobodny pr., Krasnoyarsk, Russian Federation
L.V. Kirensky Institute of Physics, 50 Akademgorodok, Krasnoyarsk, Russian Federation
Kyungpook National University, 80 Daehakro, Bukgu, Daegu, South Korea

Доп.точки доступа:
Kuzubov, A. A.; Кузубов, Александр Александрович; Kovaleva, E. A.; Avramov, P. V.; Аврамов, Павел Вениаминович; Kholtobina, A. S.; Mikhaleva, N. S.; Kuklin, A. V.; Куклин, Артем Валентинович
}
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    Carbon double coated Fe3O4@C@C nanoparticles: Morphology features, magnetic properties, dye adsorption / C. R. Lin, O. S. Ivanova, I. S. Edelman [et al.] // Nanomaterials. - 2022. - Vol. 12, Is. 3. - Ст. 376, DOI 10.3390/nano12030376. - Cited References: 44. - The work was supported financially by the Russian Foundation for Basic Research, Grant No. 19-52-52002 and Ministry of Science and Technology of Taiwan, Grants MOST No. 108-2923-M-153-001-MY3 and No. 109-2112-M-153-003-. The support was obtained also from the Joint Scientific Center of the Siberian Federal University supported by the State assignment (#FSRZ-2020-0011) of the Ministry of Science and Higher Education of the Russian Federation, where the Transmission Electron Microscopy studies were carried out . - ISSN 2079-4991
   Перевод заглавия: Наночастицы Fe3O4@C@C с двойным углеродным покрытием: Морфологические особенности, магнитные свойства, адсорбция красителей

РУБ Chemistry, Multidisciplinary + Nanoscience & Nanotechnology + Materials Science, Multidisciplinary + Physics, Applied
Рубрики:
SOLID-PHASE EXTRACTION
FE3O4 NANOPARTICLES
PROFILE REFINEMENT
Кл.слова (ненормированные):
core-shell Fe3O4@C nanoparticles -- core-shell Fe3O4@C@C nanoparticles -- magnetic properties -- dyes adsorption
Аннотация: This work is devoted to the study of magnetic Fe3O4 nanoparticles doubly coated with carbon. First, Fe3O4@C nanoparticles were synthesized by thermal decomposition. Then these synthesized nanoparticles, 20–30 nm in size were processed in a solution of glucose at 200 °C during 12 h, which led to an unexpected phenomenon – the nanoparticles self-assembled into large conglomerates of a regular shape of about 300 nm in size. The morphology and features of the magnetic properties of the obtained hybrid nanoparticles were characterized by transmission electron microscopy, differential thermo-gravimetric analysis, vibrating sample magnetometer, magnetic circular dichroism and Mössbauer spectroscopy. It was shown that the magnetic core of Fe3O4@C nanoparticles was nano-crystalline, corresponding to the Fe3O4 phase. The Fe3O4@C@C nanoparticles presumably contain Fe3O4 phase (80%) with admixture of maghemite (20%), the thickness of the carbon shell in the first case was of about 2–4 nm. The formation of very large nanoparticle conglomerates with a linear size up to 300 nm and of the same regular shape is a remarkable peculiarity of the Fe3O4@C@C nanoparticles. Adsorption of organic dyes from water by the studied nanoparticles was also studied. The best candidates for the removal of dyes were Fe3O4@C@C nanoparticles. The kinetic data showed that the adsorption processes were associated with the pseudo-second order mechanism for cationic dye methylene blue (MB) and anionic dye Congo red (CR). The equilibrium data were more consistent with the Langmuir isotherm and were perfectly described by the Langmuir–Freundlich model.

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Держатели документа:
Natl Pingtung Univ, Dept Appl Phys, Pingtung City 90003, Taiwan.
RAS, FRC KSC SB, Kirensky Inst Phys, Krasnoyarsk 660036, Russia.
Siberian Fed Univ, Inst Engn Phys & Radioelect, Krasnoyarsk 660041, Russia.
RAS, FRC KSC SB, Inst Chem & Chem Technol, Krasnoyarsk 660036, Russia.

Доп.точки доступа:
Lin, Chun-Rong; Ivanova, O. S.; Иванова, Оксана Станиславовна; Edelman, I. S.; Эдельман, Ирина Самсоновна; Knyazev, Yu. V.; Князев, Юрий Владимирович; Zharkov, S. M.; Жарков, Сергей Михайлович; Petrov, D. A.; Петров, Дмитрий Анатольевич; Sokolov, A. Е.; Соколов, Алексей Эдуардович; Svetlitsky, E. S.; Светлицкий, Евгений Сергеевич; Velikanov, D. A.; Великанов, Дмитрий Анатольевич; Solovyov, Leonid A.; Chen, Ying-Zhen; Tseng, Yaw-Teng; Russian Foundation for Basic ResearchRussian Foundation for Basic Research (RFBR) [19-52-52002]; Ministry of Science and Technology of TaiwanMinistry of Science and Technology, Taiwan [108-2923-M-153-001-MY3, 109-2112-M-153-003]; Joint Scientific Center of the Siberian Federal University [FSRZ-2020-0011]; Ministry of Science and Higher Education of the Russian Federation
}
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Cluster embedding in an elastic polarizable environment: Density functional study of Pd atoms adsorbed at oxygen vacancies of MgO(001) / V. A. Nasluzov [et al.] // J. Chem. Phys. - 2001. - Vol. 115, Is. 17. - P. 8157-8171, DOI 10.1063/1.1407001. - Cited References: 88 . - ISSN 0021-9606

РУБ Physics, Atomic, Molecular & Chemical
Рубрики:
TRANSITION-METAL ATOMS
   AB-INITIO
   OXIDE SURFACES
   ELECTRONIC-PROPERTIES
   ENERGY CALCULATIONS
   MOLECULAR-DYNAMICS
   MOTT-LITTLETON
   MADELUNG FIELD
   IONIC-CRYSTAL
   MGO
Кл.слова (ненормированные):
Atoms -- Binding energy -- Computer simulation -- Electron energy levels -- Electronic structure -- Magnesia -- Oxygen -- Palladium -- Polarization -- Probability density function -- Quantum theory -- Relaxation processes -- Charged defects -- Cluster embedding -- Elastic polarizable environment -- Electron affinity -- Oxygen vacancies -- Adsorption
Аннотация: Adsorption complexes of palladium atoms on F-s, F-s(+), F-s(2+), and O2- centers of MgO(001) surface have been investigated with a gradient-corrected (Becke-Perdew) density functional method applied to embedded cluster models. This study presents the first application of a self-consistent hybrid quantum mechanical/molecular mechanical embedding approach where the defect-induced distortions are treated variationally and the environment is allowed to react on perturbations of a reference configuration describing the regular surface. The cluster models are embedded in an elastic polarizable environment which is described at the atomistic level using a shell model treatment of ionic polarizabilities. The frontier region that separates the quantum mechanical cluster and the classical environment is represented by pseudopotential centers without basis functions. Accounting in this way for the relaxation of the electronic structure of the adsorption complex results in energy corrections of 1.9 and 5.3 eV for electron affinities of the charged defects F-s(+) and F-s(2+), respectively, as compared to models with a bulk-terminated geometry. The relaxation increases the stability of the adsorption complex Pd/F-s by 0.4 eV and decreases the stability of the complex Pd/F-s(2+) by 1.0 eV, but it only weakly affects the binding energy of Pd/F-s(+). The calculations provide no indication that the metal species is oxidized, not even for the most electron deficient complex Pd/F-s(2+). The binding energy of the complex Pd/O2- is calculated at -1.4 eV, that of the complex Pd/F-s(2+) at -1.3 eV. The complexes Pd/F-s and Pd/F-s(+) exhibit notably higher binding energies, -2.5 and -4.0 eV, respectively; in these complexes, a covalent polar adsorption bond is formed, accompanied by donation of electronic density to the Pd 5s orbital. (C) 2001 American Institute of Physics.

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Держатели документа:
Russian Acad Sci, Inst Chem & Chem Technol, Krasnoyarsk 660049, Russia
Tech Univ Munich, Inst Phys & Theoret Chem, D-85747 Garching, Germany
Kemerovo State Univ, Dept Phys, Kemerovo 650043, Russia
ИХХТ СО РАН
Institute of Chemistry and Chemical Technology, Russian Academy of Sciences, 660049 Krasnoyarsk, Russian Federation
Institut fur Physikalische und Theoretische Chemie, Technische Universitat Munchen, 85747 Garching, Germany

Доп.точки доступа:
Nasluzov, V. A.; Rivanenkov, V. V.; Gordienko, A. B.; Neyman, K. M.; Birkenheuer, U.; Rosch, N.
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Core-shell magnetite nanoparticles: morphology, magnetic properties, organic dyes adsorption / O. S. Ivanova, I. S. Edelman, E. S. Svetlitsky [et al.] // International conference "Functional materials" : book of abstracts / ed. V. N. Berzhansky ; org. com. S. G. Ovchinnikov [et al.]. - Simferopol, 2023. - P. 114. - Cited References: 1. - РФН № 23-22-10025

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Держатели документа:
Kirensky Institute of Physics, FRC KSC SB RAS,
Siberian Federal University
National Pingtung University, 90003, Pingtung City, Taiwan

Доп.точки доступа:
Berzhansky, V. N. \ed.\; Бержанский, Владимир Наумович; Ovchinnikov, S. G. \org. com.\; Овчинников, Сергей Геннадьевич; Ivanova, O. S.; Иванова, Оксана Станиславовна; Edelman, I. S. (Edel'man, I. S.); Эдельман, Ирина Самсоновна; Svetlitsky, E. S.; Sokolov, A. Е.; Соколов, Алексей Эдуардович; Zharkov, S. M.; Жарков, Сергей Михайлович; Petrov, D. A.; Петров, Дмитрий Анатольевич; Sukhachev, A. L.; Сухачев, Александр Леонидович; Toropova, E. S.; Chun-Rong Lin; Ying-Zhen Chen; "Functional materials", International conference(2023 ; Oct. 2-6 ; Crimea, Foros); Крымский федеральный университет имени В.И. Вернадского
}
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Core–shell Fe3O4@C nanoparticles for the organic dye adsorption and targeted magneto-mechanical destruction of Ehrlich ascites carcinoma cells / O. S. Ivanova, I. S. Edelman, Ch.-R. Lin [et al.] // Materials. - 2023. - Vol. 16, Is. 1. - Ст. 23, DOI 10.3390/ma16010023. - Cited References: 65. - This research was funded partly by the Ministry of Science and Higher Education of the Russian Federation, project FWES-2021-0035. C.-R.L., Y.-Z.C. and A.A.S. thank the National Science and Technology Council of Taiwan for the financial support, Grants NSTC № 108-2923-M-153-001-MY3 and № 110-2112-M-153-005-. Magnetic investigations were carried out in the Center for Collective Use of the Krasnoyarsk Regional Center of Research Equipment of Federal Research Center “Krasnoyarsk Science Center SB RAS” . - ISSN 1996-1944
Кл.слова (ненормированные):
magnetite nanoparticles -- adsorption -- organic dyes -- aptamers -- magnetically induced cell destruction
Аннотация: The morphology, structure, and magnetic properties of Fe3O4 and Fe3O4@C nanoparticles, as well their effectiveness for organic dye adsorption and targeted destruction of carcinoma cells, were studied. The nanoparticles exhibited a high magnetic saturation value (79.4 and 63.8 emu/g, correspondingly) to facilitate magnetic separation. It has been shown that surface properties play a key role in the adsorption process. Both types of organic dyes—cationic (Rhodomine C) and anionic (Congo Red and Eosine)—were well adsorbed by the Fe3O4 nanoparticles’ surface, and the adsorption process was described by the polymolecular adsorption model with a maximum adsorption capacity of 58, 22, and 14 mg/g for Congo Red, Eosine, and Rhodomine C, correspondingly. In this case, the kinetic data were described well by the pseudo-first-order model. Carbon-coated particles selectively adsorbed only cationic dyes, and the adsorption process for Methylene Blue was described by the Freundlich model, with a maximum adsorption capacity of 14 mg/g. For the case of Rhodomine C, the adsorption isotherm has a polymolecular character with a maximum adsorption capacity of 34 mg/g. To realize the targeted destruction of the carcinoma cells, the Fe3O4@C nanoparticles were functionalized with aptamers, and an experiment on the Ehrlich ascetic carcinoma cells’ destruction was carried out successively using a low-frequency alternating magnetic field. The number of cells destroyed as a result of their interaction with Fe3O4@C nanoparticles in an alternating magnetic field was 27%, compared with the number of naturally dead control cells of 6%.

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Держатели документа:
Kirensky Institute of Physics, Federal Research Center KSC Siberian Branch, Russian Academy of Sciences, Krasnoyarsk 660036, Russia
Institute of Engineering Physics and Radioelectronics, Siberian Federal University, Krasnoyarsk 660041, Russia
Department of Applied Physics, National Pingtung University, Pingtung City 90003, Taiwan
Laboratory of Biomolecular and Medical Technologies, Krasnoyarsk State Medical University Named after Prof. V.F. Voino-Yasenetsky, Krasnoyarsk 660022, Russia
Laboratory for Digital Controlled Drugs and Theranostics, Federal Research Center KSC Siberian Branch, Russian Academy of Sciences, Krasnoyarsk 660036, Russia

Доп.точки доступа:
Ivanova, O. S.; Иванова, Оксана Станиславовна; Edelman, I. S.; Эдельман, Ирина Самсоновна; Lin, Chun-Rong; Svetlitsky, E. S.; Светлицкий, Евгений Сергеевич; Sokolov, A. Е.; Соколов, Алексей Эдуардович; Lukyanenko, Kirill A.; Sukhachev, A. L.; Сухачев, Александр Леонидович; Shestakov, N. P.; Шестаков, Николай Петрович; Chen, Ying-Zhen; Spivakov, Aleksandr A.
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10.

Crystal size: Versus paddle wheel deformability: Selective gated adsorption transitions of the switchable metal-organic frameworks DUT-8(Co) and DUT-8(Ni) / S. Ehrling [et al.] // J. Mater. Chem. A. - 2019. - Vol. 7, Is. 37. - P. 21459-21475, DOI 10.1039/c9ta06781g. - Cited References: 106. - The authors thank DFG (FOR 2433) for financial support. We thank HZB for the allocation of synchrotron radiation beam-time and financial support. PP, TW and TH used high performance facilities of ZIH Dresden. TW thanks the European Social Funds for Germany for a PhD fellowship. . - ISSN 2050-7488
Кл.слова (ненормированные):
Cobalt -- Crystallite size -- Density functional theory -- Dichloromethane -- Inclusions -- Nickel -- Organometallics -- Particle size -- Physisorption -- Single crystals -- Wheels -- X ray powder diffraction
Аннотация: Switchable pillared layer metal–organic frameworks M2(2,6-ndc)2(dabco) (DUT-8(M), M = Ni, Co, 2,6-ndc = 2,6-naphthalenedicarboxylate, dabco = 1,4-diazabicyclo-[2.2.2]octane, DUT – Dresden University of Technology) were synthesised in two different crystallite size regimes to produce particles up to 300 μm and smaller particles around 0.1 μm, respectively. The textural properties and adsorption-induced switchability of the materials, obtained from both syntheses, were studied by physisorption of N2 at 77 K, CO2 at 195 K and n-butane at 273 K, revealing pronounced differences in adsorption behavior for Ni and Co analogues. While the smaller nano-sized particles (50–200 nm) are rigid and show no gating transitions confirming the importance of crystallite size, the large particles show pronounced switchability with characteristic differences for the two metals resulting in distinct recognition effects for various gases and vapours. Adsorption of various vapours demonstrates consistently a higher energetic barrier for the “gate opening” of DUT-8(Co) in contrast to DUT-8(Ni), as the “gate opening” pressure for Co based material is shifted to a higher value for adsorption of dichloromethane at 298 K. Evaluation of crystallographic data, obtained from single crystal and powder X-ray diffraction analysis, showed distinct geometric differences in the paddle wheel units of the respective MOFs. These differences are further disclosed by solid-state UV-vis, FT-IR and Raman spectroscopy. Magnetic properties of DUT-8(Co) and DUT-8(Ni) were investigated, indicating a high-spin state for both materials at room temperature. Density functional theory (DFT) simulations confirmed distinct energetic differences for Ni and Co analogues with a higher energetic penalty for the structural “gate opening” transformation for DUT-8(Co) compared to DUT-8(Ni) explaining the different flexibility behaviour of these isomorphous MOFs.

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Держатели документа:
Department of Inorganic Chemistry, Technische Universitat Dresden, Bergstrasse 66, Dresden, 01069, Germany
University of Sofia, Faculty of Chemistry and Pharmacy, Sofia, 1126, Bulgaria
Leibniz Institute for Solid State and Materials Research, IFW Dresden, Helmholtz-strasse 20, Dresden, 01069, Germany
Wilhelm-Ostwald-Institute of Physical and Theoretical Chemistry, Faculty for Chemistry and Mineralogy, Leipzig University, Leipzig, 04103, Germany
Helmholtz-Zentrum Dresden-Rossendorf, Institute of Resource Ecology, Research Site Leipzig, Permoserstr. 15, Leipzig, 04318, Germany
Kirensky Institute of Physics, Federal Research Center KSC SB RAS, Krasnoyarsk, 660036, Russian Federation
Siberian Federal University, Svobodny Prospect 79, Krasnoyarsk, 660041, Russian Federation
Institute of Automation and Electrometry of the SB RAS, Novosibirsk, 630090, Russian Federation
Research Group Macromolecular Crystallography, Helmholtz-Zentrum Berlin fur Materialien und Energie, Albert-Einstein-Stra?e 15, Berlin, 12489, Germany
Department of Theoretical Chemistry, Technische Universitat Dresden, Berg-strasse 66, Dresden, 01069, Germany

Доп.точки доступа:
Ehrling, S.; Senkovska, I.; Bon, V.; Evans, J. D.; Petkov, P.; Krupskaya, Y.; Kataev, V.; Wulf, T.; Krylov, A. S.; Крылов, Александр Сергеевич; Vtyurin, A. N.; Втюрин, Александр Николаевич; Krylova, S. N.; Крылова, Светлана Николаевна; Adichtchev, S.; Slyusareva, E.; Weiss, M. S.; Buchner, B.; Heine, T.; Kaskel, S.
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