Publications 2016

Scientific Publications of the CINN in 2016

19

Dec 2016

Nucleophilic Additions to Coordinated 1,10-Phenanthroline: Intramolecular, Intermolecular, Reversible, and Irreversible

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KN(SiMe3)2 reacts with [Re(CO)3(phen)(PMe3)]OTf via reversible addition to the phen ligand and irreversible deprotonation of the PMe3 ligand followed by intramolecular attack to phen by the deprotonated phosphane, whereas MeLi irreversibly adds to phen. The addition of MeLi has been shown to be intermolecular, unlike previously known nucleophilic additions to pyridines.

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02

Dec 2016

The effect of exposure to nanoparticles and nanomaterials on the mammalian epigenome

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Human exposure to nanomaterials and nanoparticles is increasing rapidly, but their effects on human health are still largely unknown. Epigenetic modifications are attracting ever more interest as possible underlying molecular mechanisms of gene–environment interactions, highlighting them as potential molecular targets following exposure to nanomaterials and nanoparticles. Interestingly, recent research has identified changes in DNA methylation, histone post-translational modifications, and noncoding RNAs in mammalian cells exposed to nanomaterials and nanoparticles. However, the challenge for the future will be to determine the molecular pathways driving these epigenetic alterations, the possible functional consequences, and the potential effects on health.

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02

Dec 2016

Activation of Aromatic C−C Bonds of 2,2’-Bipyridine Ligands

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4,4’-Disubstituted- 2,2′-bipyridine ligands coordinated to MoII and ReI cationic fragments become dearomatized by an intramolecular nucleophilic attack from a deprotonated N-alkylimidazole ligand in cis disposition. The subsequent protonation of these neutral complexes takes place on a pyridine carbon atom rather than at nitrogen, weakening an aromatic C−C bond and affording a dihydropyridyl moiety. Computational calculations allowed for the rationalization of the formation of the experimentally obtained products over other plausible alternatives.

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28

Nov 2016

Specifics of Wear of Ceramic Cutting Tool Inserts Featuring Al2O3-TiC Dies when Face Milling Hardened Cast Iron

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This work studies wear kinetics of index able inserts (II) made of mixed ceramics based on Russian-manufactured in case of fine milling of special hardened cast iron with globular graphite. In a wide range of cutting parameters typical for fine milling, an impact of tool insert wearing parameters on qualitative and quantitative characteristics of the cutting process have been studied. Morphological traits and nature of wear of work surfaces has been studied using optical and scanning electron microscopy. Criteria of II states, as well as specifics of contact work surface transformation, correlating with force parameters of the face milling process, have been determined.

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07

Nov 2016

Differentiation of Mouse Embryonic Stem Cells Toward Functional Pancreatic β-Cell Surrogates Through Epigenetic Regulation of Pdx1 by Nitric Oxide

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Pancreatic and duodenal homeobox 1 (Pdx1) is a transcription factor that regulates the embryonic development of the pancreas and the differentiation toward β cells. Previously, we have shown that exposure of mouse embryonic stem cells (mESCs) to high concentrations of diethylenetriamine nitric oxide adduct (DETA-NO) triggers differentiation events and promotes the expression of Pdx1. Here we report evidence that Pdx1 expression is associated with release of polycomb repressive complex 2 (PRC2) and P300 from its promoter region. These events are accompanied by epigenetic changes in bivalent markers of histones trimethylated histone H3 lysine 27 (H3K27me3) and H3K4me3, site-specific changes in DNA methylation, and no change in H3 acetylation. On the basis of these findings, we developed a protocol to differentiate mESCs toward insulin-producing cells consisting of sequential exposure to DETA-NO, valproic acid, and P300 inhibitor (C646) to enhance Pdx1 expression and a final maturation step of culture in suspension to form cell aggregates. This small molecule-based protocol succeeds in obtaining cells that express pancreatic β-cell markers such as PDX1, INS1, GCK, and GLUT2 and respond in vitro to high glucose and KCl.

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07

Nov 2016

Development Refractoriness of MLL-Rearranged Human B Cell Acute Leukemias to Reprogramming into Pluripotency

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Induced pluripotent stem cells (iPSCs) are a powerful tool for disease modeling. They are routinely generated from healthy donors and patients from multiple cell types at different developmental stages. However, reprogramming leukemias is an extremely inefficient process. Few studies generated iPSCs from primary chronic myeloid leukemias, but iPSC generation from acute myeloid or lymphoid leukemias (ALL) has not been achieved. We attempted to generate iPSCs from different subtypes of B-ALL to address the developmental impact of leukemic fusion genes. OKSM(L)-expressing mono/polycistronic-, retroviral/lentiviral/episomal-, and Sendai virus vector-based reprogramming strategies failed to render iPSCs in vitro and in vivo. Addition of transcriptomic-epigenetic reprogramming “boosters” also failed to generate iPSCs from B cell blasts and B-ALL lines, and when iPSCs emerged they lacked leukemic fusion genes, demonstrating non-leukemic myeloid origin. Conversely, MLL-AF4-overexpressing hematopoietic stem cells/B progenitors were successfully reprogrammed, indicating that B cell origin and leukemic fusion gene were not reprogramming barriers. Global transcriptome/DNA methylome profiling suggested a developmental/differentiation refractoriness of MLL-rearranged B-ALL to reprogramming into pluripotency.

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31

Oct 2016

Crystal structure of N′-[(1E)-(2,6-dichlorophenyl)-methylidene]adamantane-1-carbohydrazide, C18H20Cl2N2O

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C18H20Cl2N2O, orthorhombic, Pbca (No. 61), a = 8.1023(2) Å, b = 18.7063(4) Å, c = 22.5509(6) Å, V = 3417.91(14) Å3, Z = 8, Rgt(F) = 0.0496, wRref(F2) = 0.1535, T = 293(2).

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31

Oct 2016

Broadband dielectric spectroscopy of standard and core-shell BaTiO3-NiO ceramic composites compared to the BaTiO3 ceramics

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Using spark plasma sintering we have processed and studied two ceramic composites of 70 vol% BaTiO3(BTO) and 30 vol% NiO with different topologies: standard and core-shell composites. The materials were characterized by X-ray diffraction and scanning electron microscopy and studied by quantitative broadband dielectric spectroscopy up to the infrared range using four different spectroscopic techniques in the 10-450 K temperature range. The spectra, which differed quite appreciably from each other, were fitted with the factorized dielectric function of generalized damped oscillators in the infrared-terahertz range and by a set of Cole-Cole relaxations at lower frequencies below the polar phonon frequency range. All three ferroelectric phase transitions were indicated by the maxima in the temperature dependent low-frequency permittivity, with no temperature shift compared to BTO. Using the dielectric functions of the BTO ceramics and NiO crystal, we modelled the effective dielectric functions of the composite using three models based on the effective medium approximation: Bruggeman, Lichtenecker and generalized brick model (coated spheres). The models were discussed on the basis of the degree of BTO-grain percolation through the composite, which strongly affects the effective BTO soft-mode behaviour. Qualitative agreement between the experimental and modelled effective dielectric functions was obtained, but small discrepancies indicate some interdiffusion between the BTO grains and NiO shells, which also affected the rather complex dielectric dispersion and conductivity spectra below the phonon frequency range.

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21

Oct 2016

Temperature-Dependent Supramolecular Isomerism of Lutetium-Aminoterephthalate Metal–Organic Frameworks: Synthesis, Crystallography, and Physical Properties

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Three supramolecular isomers of lutetium metal–organic framework, {Lu2(H2O)4(ATA)3·4H2O}n(Lu-ATA@RT), {Lu2(H2O)2(C3H7NO)2(ATA)3}n (Lu-ATA@100), and {Lu2(C3H7NO)(ATA)3}n (Lu-ATA@150), have been obtained from the reaction of Lu(NO3)3·6H2O with 2-aminoterephthalic acid (ATA) at different temperatures. The resulting structures of Lu-ATA metal–organic frameworks depend on the temperature applied during the synthesis, revealing a temperature-susceptible supramolecular isomerism. Single-crystal X-ray diffraction analyses suggest that new compounds with formula {Lu2(S)x(ATA)3}n (S = solvent: H2O, DMF) display different three-dimensional architectures which consist of dinuclear lutetium building units. The supramolecular isomer Lu-ATA@RT, formed at room temperature, has a pcu-net topology, while its double interpenetrated analogue Lu-ATA@100 assembles at 100 °C under hydrothermal conditions. Hydrothermal synthesis at 150 °C affords formation of the dense Lu-ATA@150 cage-like framework displaying a new hexagonal-packed net topology. All Lu-ATA isomeric phases are porous and display different gas-uptake behavior toward carbon dioxide as a function of polymeric network arrangement. The luminescent properties of Lu-ATA frameworks in the solid state as well as in suspension in the presence of different solvents reveal a solvent-dependent emission.

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09

Oct 2016

Antimicrobial activity of submicron glass fibres incorporated as a filler to a dental sealer

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Two types of antimicrobial glass fibers containing ZnO and CaO, with diameters ranging from tens of nanometers to 1 µm, were successfully fabricated by a laser spinning technique. The antimicrobial performance was corroborated according to ISO 20743:2013, by using gram-negative (Escherichia coli) and gram-positive (Streptococcus oralis, Streptococcus mutans and Staphylococcus aureus) bacteria, and yeast (Candida krusei) (more than 3 logs of reduction). The metabolic activity and endosomal system of eukaryotic cells were not altered by using eluents of CaO glass submicrometric fibers and ZnO fibers at 1 : 10 dilution as cellular media (viability rates over 70%). A dental material was functionalized by embedding ZnO nanofibers above the percolation threshold (20% wt), creating a three-dimensional (3D) fiber network that added an antimicrobial profile. This new ZnO glass fiber composite is proved non-cytotoxic and preserved the antimicrobial effect after immersion in human saliva. This is the first time that a fiber-reinforced liner with strong antimicrobial-activity has been created to prevent secondary caries. The potential of developing new fiber-reinforced composites (FRCs) with antimicrobial properties opens up an extensive field of dental applications where most important diseases have an infectious origin.

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