256 research outputs found

    Azine Activation via Silylium Catalysis

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    Practical, efficient, and general methods for the diversification of N-heterocycles have been a recurrent goal in chemical synthesis due to the ubiquitous influence of these motifs within bioactive frameworks. Here, we describe a direct, catalytic, and selective functionalization of azines via silylium activation. Our catalyst design enables mild conditions and a remarkable functional group tolerance in a one-pot setup

    Intriguing mechanistic labyrinths in gold(I) catalysis

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    Many mechanistically intriguing reactions have been developed in the last decade using gold(I) as catalyst. Here we review the main mechanistic proposals in gold-catalysed activation of alkynes and allenes, in which this metal plays a central role by stabilising a variety of complex cationic intermediates

    Surface charge reversal method for high-resolution inkjet printing of functional water-based inks

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    © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. Printed electronics is a rapidly growing area of research being explored for the manufacture of large-area and cost-effective electronic devices by the patterned application of functional inks. There are challenges associated with processing the inks compatible with inkjet printing technology and developing effi cient methods to successfully obtain the desired features, particularly when it comes to metal and metal-organic complex inks. Here, a reliable method is developed to achieve a sophisticated microstructured pattern using the inkjet printing technique assisted by a surface charge reversal effect. In addition, a procedure is formulated to obtain good quality, stable metal-organic water-based inks compatible with salts of a variety of transition metals and rare earths, without the need for additional volatile solvents. A feasible and water-based ink formulation combined with a simple and noninvasive surface charge reversal treatment constitutes a major step toward the manufacture of high-resolution, inorganic patterned thin fi lms on hydrophobic substrates using inkjet printing. These outcomes lead to the path of effective fusion of inorganic and organic heterointerfaces by simples designing and printing.This work was supported by the University of New South Wales and Spanish MICINN (Consolider CSD2007-0041). A portion of this work was performed at the ACT node of the Australian National Fabrication Facility. The authors wish to acknowledge Dr. F. Kremer for the electron diffraction measurement.Peer Reviewe

    Direct and Catalytic C-Glycosylation of Arenes: Expeditious Synthesis of the Remdesivir Nucleoside

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    Since early 2020, scientists have strived to find an effective solution to fight SARS-CoV-2, especially by developing reliable vaccines that inhibit the spread of the disease and repurposing drugs for combatting its effects on the human body. The antiviral prodrug Remdesivir is still the most widely used therapeutic during the early stage of the infection. However, the current synthetic routes rely on the use of protecting groups, air-sensitive reagents, and cryogenic conditions, impeding the cost-efficient supply to patients. We therefore focused on the development of a straightforward, direct addition of (hetero)arenes to unprotected sugars. Here we report a silylium-catalyzed and completely stereoselective C -glycosylation that initially yields the open-chain polyols, which can be selectively cyclized to provide either the kinetic α-furanose or the thermodynamically favored β-anomer. The method significantly expedites the synthesis of Remdesivir precursor GS-441524 after subsequent Mn-catalyzed C–H oxidation and deoxycyanation

    A hidden Goldstone mechanism in the Kagom\'e lattice antiferromagnet

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    In this paper, we study the phases of the Heisenberg model on the \kagome lattice with antiferromagnetic nearest neighbour coupling J1J_1 and ferromagnetic next neighbour coupling J2J_2. Analysing the long wavelength, low energy effective action that describes this model, we arrive at the phase diagram as a function of χ=J2J1\chi = \frac{J_2}{J_1} . The interesting part of this phase diagram is that for small χ\chi, which includes χ=0\chi =0, there is a phase with no long range spin order and with gapless and spin zero low lying excitations. We discuss our results in the context of earlier, numerical and experimental work.Comment: 21 pages, latex file with 5 figure

    Observation of insulator-metal transition in EuNiO3_{3} under high pressure

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    The charge transfer antiferromagnetic (TN_{N} =220 K) insulator EuNiO3_{3} undergoes, at ambient pressure, a temperature-induced metal insulator MI transition at TMI_{MI}=463 K. We have investigated the effect of pressure (up to p~20 GPa) on the electronic, magnetic and structural properties of EuNiO3_{3} using electrical resistance measurements, {151}^Eu nuclear resonance scattering of synchrotron radiation and x-ray diffraction, respectively. With increasing pressure we find at pc_{c} =5.8 GPa a transition from the insulating state to a metallic state, while the orthorhombic structure remains unchanged up to 20 GPa. The results are explained in terms of a gradual increase of the electronic bandwidth with increasing pressure, which results in a closing of the charge transfer gap. It is further shown that the pressure-induced metallic state exhibits magnetic order with a lowervalue of TN_{N} (TN_{N} ~120 K at 9.4 GPa) which disappears between 9.4 and 14.4 GPa.Comment: 10 pages, 3 figure

    Complejos de cefalexina con cationes de elementos del cuarto periodo. I.-Estudio en disolución acuosa

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    The formation of the complexes, in aqueous solution, between the cephalexin and sorne ious of the fourth period elements has been investigated by potentiometric and spectrophotometric methods. The stability constants has been determinated.Se ha investigado la formación de complejos, en disolución acuosa, de cefalexina [ácido 7-(D-2-amino-2-fenil-acetamido )-3-metil-8-oxo-S-tia-1-azabiciclo [4.2.O] oct-2-eno-2-carboxilico] con cationes de elementos del cuarto período, por métodos potenciométricos y espectrofotométricos. Se han determinado asímismo las constantes de formación de complejos

    Finite-Temperature Transition into a Power-Law Spin Phase with an Extensive Zero-Point Entropy

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    We introduce an xyxy generalization of the frustrated Ising model on a triangular lattice. The presence of continuous degrees of freedom stabilizes a {\em finite-temperature} spin state with {\em power-law} discrete spin correlations and an extensive zero-point entropy. In this phase, the unquenched degrees of freedom can be described by a fluctuating surface with logarithmic height correlations. Finite-size Monte Carlo simulations have been used to characterize the exponents of the transition and the dynamics of the low-temperature phase
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