986 research outputs found

    Relations between personality changes and cerebrospinal fluid biomarkers of Alzheimer's disease pathology.

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    Specific changes in personality profiles may represent early non-cognitive symptoms of Alzheimer's disease (AD). Evaluating the subject's personality changes may add significant clinical information, as well as help to better understand the interaction between personality change, cognitive decline, and cerebral pathology. With this study we aimed to describe the relationship between personality changes and cerebrospinal fluid (CSF) markers of AD pathology at early clinical stages of the disease. One hundred and ten subjects, of whom 66 cognitively impaired patients (57 with mild cognitive impairment (MCI), and 9 with mild dementia) and 44 healthy controls, had neuropsychological examination as well as lumbar puncture to determine concentrations of CSF biomarkers of AD pathology (amyloid beta javax.xml.bind.JAXBElement@6dd80402 (Aβ javax.xml.bind.JAXBElement@750f1490 ), phosphorylated tau (ptau-181), and total-tau (tau)). The Revised NEO Personality Inventory (NEO-PI-R) was administered twice, once to evaluate subjects' current personality and once to assess personality traits retrospectively 5 years before evaluation. Subjects with an AD CSF biomarker profile showed significant increase in neuroticism and decrease in conscientiousness over time as compared to non-AD CSF biomarker group. In regression analysis controlling for global cognition as measured by the MMSE score, increasing neuroticism and decreasing extraversion, openness to experience and conscientiousness were associated with lower Aβ javax.xml.bind.JAXBElement@71367816 concentrations but not with tau and ptau-181 concentrations. Our findings suggest that early and specific changes in personality are associated with cerebral AD pathology. Concentrations of CSF biomarkers, additionally to severity of the cognitive impairment, significantly contribute in predicting specific personality changes

    Microwave-irradiated rapid synthesis of antimicrobial pyrazine derivatives in reactive eutectic media

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    Herein, we report of the use of reactive eutectic media from ammonium formate and monosaccharides to synthesize poly(hydroxyalkyl)pyrazines via microwave irradiation. This enabled unprecedented fast rates as well as better atom economy compared to previous methods. We investigated the influence of water on the reaction yield as well as the physical properties of the eutectic media and could thereby drastically reduce the viscosity, while preserving high reaction yields. The results were consistent for different monosaccharide, using fructose, glucose, rhamnose and fucose as reactants. Furthermore, the major reaction products were separated, chemically analyzed and tested on their antimicrobial activity via high-throughput screening

    A tale of two membranes: from poly(ionic liquid) to metal-organic framework hybrid nanoporous membranes via pseudomorphic replacement

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    A general approach to produce a variety of free-standing asymmetric MOF hybrid membranes and superstructure arrays on "inert" substrates with tailored crystal sizes and shapes was developed. The obtained MOF hyrid membrane exhibits fast actuation in response to external gas stimulus

    Saving the energy loss in lithium-mediated nitrogen fixation by using highly reactive Li<sub>3</sub>N intermediate for C–N coupling reactions

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    Direct synthesis of N-containing organic compounds from dinitrogen (N2) can make synthetic chemistry more sustainable. Previous bottlenecks in lithium-mediated N2 fixation were resolved by loading Li metal anodes covered with the typical Li+ ion-conducting solid electrolyte interface, which are subsequently allowed to react with N2. The developed strategy allowed us to reach high Faradaic efficiencies toward Li3N. These reactive Li3N were then contacted with acylchlorides. Surface nitride ions are more nucleophilic than amines which direct the two C–N coupling reactions toward formation of imides rather than amides, and an integrated current efficiency of 57~77% could be realized. This study thereby not only provides a feasible electrochemical Li3N synthesis, but also delineates an economical and green synthesis of highly valuable N-containing compounds from N2 under mild conditions, just using commercial spare parts and processes from omnipresent Li battery technology

    Activating cobalt nanoparticles via the Mott-Schottky effect in nitrogen-rich carbon shells for base-free aerobic oxidation of alcohols to esters

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    Heterogeneous catalysts of inexpensive and reusable transition-metal are attractive alternatives to homogeneous cat-alysts; the relatively low activity of transition-metal nanoparticles has become the main hurdle for their practical ap-plications. Here, the de novo design of a Mott-Schottky-type heterogeneous catalyst is reported to boost the activity of a transition-metal nanocatalyst through electron transfer at the metal/nitrogen-doped carbon interface. The Mott-Schottky catalyst of nitrogen-rich carbon-coated cobalt nanoparticles (Co@NC) was prepared through direct polycon-densation of simple organic molecules and inorganic metal salts in the presence of g-C3N4 powder. The Co@NC with controllable nitrogen content and thus tunable Fermi energy and catalytic activity exhibited a high turnover frequency (TOF) value (8.12 mol methyl benzoate mol-1 Co h-1) for the direct, base-free, aerobic oxidation of benzyl alcohols to methyl benzoate; this TOF is 30-fold higher than those of the state-of-the-art transition-metal-based nanocatalysts reported in the literature. The presented efficient Mott-Schottky catalyst can trigger the synthesis of a series of alkyl esters and even diesters in high yields

    A Cu(ii) metal-organic framework as a recyclable catalyst for ARGET ATRP

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    A Cu(ii) MOF can serve as an efficient catalyst for activators regenerated by electron transfer atom transfer radical polymerization (ARGET ATRP), e.g. for the synthesis of poly(benzyl methacrylate) (PBzMA) and polystyrene (PS). Furthermore, poly(isoprene) (PI) and poly(4-vinylpyridine) (P4VP) can be formed in a controlled fashion as well, which used to be challenging to achieve by traditional strategies. Taking advantage of the heterogeneous nature of the catalyst, recycling via centrifugation and repeated utilization for at least six cycles are demonstrated

    A General Synthetic Route Towards Highly Dispersed Metal Clusters Enabled by Poly ionic liquid s

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    The ability to synthesize a broad spectrum of metal clusters MCs with their size controllable on a subnanometer scale presents an enticing prospect for exploring nanosize dependent properties. Here we report an innovative design of a capping agent from a polytriazolium poly ionic liquid PIL in a vesicular form in solution that allows for crafting a variety of MCs including transition metals, noble metals, and their bimetallic alloy with precisely controlled sizes amp; 8764;1 nm and record high catalytic performance. The ultrastrong stabilization power is a result of an unusual synergy between the conventional binding sites in the heterocyclic cations in PIL and an in situ generated polycarbene structure induced simultaneously to the reduction reactio

    Review of discontinuous Galerkin finite element methods for partial differential equations on complicated domains

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    The numerical approximation of partial differential equations (PDEs) posed on complicated geometries, which include a large number of small geometrical features or microstructures, represents a challenging computational problem. Indeed, the use of standard mesh generators, employing simplices or tensor product elements, for example, naturally leads to very fine finite element meshes, and hence the computational effort required to numerically approximate the underlying PDE problem may be prohibitively expensive. As an alternative approach, in this article we present a review of composite/agglomerated discontinuous Galerkin finite element methods (DGFEMs) which employ general polytopic elements. Here, the elements are typically constructed as the union of standard element shapes; in this way, the minimal dimension of the underlying composite finite element space is independent of the number of geometrical features. In particular, we provide an overview of hp-version inverse estimates and approximation results for general polytopic elements, which are sharp with respect to element facet degeneration. On the basis of these results, a priori error bounds for the hp-DGFEM approximation of both second-order elliptic and first-order hyperbolic PDEs will be derived. Finally, we present numerical experiments which highlight the practical application of DGFEMs on meshes consisting of general polytopic elements

    Cu<sup>II</sup>/Cu<sup>I</sup> decorated N-doped carbonaceous electrocatalysts for the oxygen reduction reaction

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    The oxygen reduction reaction (ORR) that for instance takes place at the cathode of fuel cells is one of the most examined model reactions of energy conversion. The ORR presents sluggish reaction kinetics, thus limiting the overall efficiency of these cells. Pt-based catalysts are still the widest choice though they exhibit important drawbacks such as long-term instability and intolerance to methanol crossover. In this context, engineering transition metals in the form of nano- and subnano-sites on carbonaceous supports has the potential of becoming an alternative to scarce noble metal-based catalysts. Herein, we describe a simple synthetic route towards CuII/CuI decorated N-doped carbonaceous ORR electrocatalysts. CuII/CuI nanosites are obtained by calcination in air of an ionic liquid derived noble carbonaceous support impregnated with copper(ii) acetate. The strong interaction between the copper and the noble support foster the co-formation of CuII/CuI nanosites. Larger amounts of copper(ii) acetate translate into larger amounts of CuI and lower Tafel slopes. The material with 4 wt% of copper catalyzes the selective reduction of oxygen through a 4-electron transfer pathway and exhibits a lower Tafel slope than commercial platinum, a minimal overpotential, and a higher limiting current density. Moreover, all materials show promising durability and high methanol stability, which makes them promising to replace noble metals for the ORR
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