6,311 research outputs found

    Heterogeneous PdAg alloy catalyst for selective methylation of aromatic amines with formic acid under an additive-free and solvothermal one-pot condition

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    The methylation of amines for the synthesis of methylamines and dimethylamines as platform chemicals has been attempted mostly by homogeneous catalysts with acid additives. However, there are scarcely any reports on heterogeneous catalytic methylation reactions except for a routine approach under high temperature and high pressure of CO2 and H-2 gases for extended reaction times. Here we report a heterogeneously catalyzed selective methylation of aromatic amines using reactive and nontoxic formic acid as the only source for the construction of methyl groups, under ambient pressure in an additive-free one-pot reaction condition. Equal proportions of Pd and Ag in the PdAg/Fe3O4/N-rGO catalyst deliver highly selective amine methylation without aromatic ring hydrogenation, as the strained Pd in the alloy is combined with the graphene-derived support, preventing nanoparticle agglomeration and the action of magnetite as a promoter. Both N-methylation and N, N-dimethylation of various substituted aromatic amines were performed with complete conversion and excellent 90-97% selectivity by controlling the reaction times in the range of 10-24 h at 140 degrees C without unwanted aromatic ring hydrogenation. Furthermore, the developed bimetallic catalyst provided high yields (88-91%) of methylation with CO2+H-2 gas under high pressure, which are as good as the results of homogenous catalysts with an acid additive. To the best of our knowledge, our use of this environmentally friendly methodology is the first time that this durable heterogeneous catalyst has readily performed highly selective methylation at ambient pressure, which is attractive for industrial applications.1193Ysciescopu

    How willing are you to accept sexual requests from slightly unattractive to exceptionally attractive imagined requestors?

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    This is the post print version of the article. The official published version can be accessed from the link below.In their classic study of differences in mating strategies (Clark & Hatfield, 1989), men and women demonstrated a striking difference in interest in casual sex. The current study examined the role of requestor physical attractiveness (slightly unattractive, moderately attractive and exceptionally attractive) on men's and women's willingness to accept three different requests (go out, come to apartment, go to bed) in a questionnaire study. We tested two hypotheses, using a sample of 427 men and 443 women from three countries. Hypothesis 1 states that men, relative to women, will demonstrate a greater willingness to accept the “come to apartment” and “go to bed” requests but not the “go out” request for all three levels of requestor attractiveness. This hypothesis reflects Clark and Hatfield's (1989) main findings. Hypothesis 2 states that the physical attractiveness of a potential partner will have a greater effect on women's than on men's willingness to accept all three requests, and particularly for the explicit request for casual sex. The results partially supported Hypothesis 1 and fully supported Hypothesis 2. The discussion highlights limitations of the current research and presents directions for future research

    One-flow Syntheses of Diverse Heterocyclic Furan Chemicals Directly from Fructose via Tandem Transformation Platform

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    The sustainable green chemistry associated with lignocellulosic biomass is of current interest for producing various chemical feedstocks via multi-step transformation processes. Here we introduce a chemical platform system for the multicomponent cascade transformation of natural lignocellulosic biomass resources. We demonstrate the concept by developing an integrated continuous two-step microfluidic system as a tandem transformation platform for direct conversion of fructose to diverse furan chemicals with excellent yields up to 99% via decarbonylation, etherification, oxidation and hydrogenolysis of a 5-hydroxymethylfurfural (HMF) intermediate. A sequential two-step process is utilized to complete the dehydration of fructose in the surface acid catalyst at 150 degrees C for 6 min, which is followed by the four types of HMF conversion in a binary or ternary phase to produce furfuryl alcohol (94% yield), 5-ethoxymethylfurfural (99%), 2,5-diformylfuran (82%) and 2,5-dimethylfuran (90%) with magnetic-based heterogeneous catalysts at 70-150 degrees C for 6-60 min. This innovative tandem microfluidic platform enables precise control of the reaction temperature and time for each individual biomass conversion step in a one-flow manner with no separation and purification steps for intermediates and catalysts.112016Ysciescopu

    Micro-total envelope system with silicon nanowire separator for safe carcinogenic chemistry

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    Exploration and expansion of the chemistries involving toxic or carcinogenic reagents are severely limited by the health hazards their presence poses. Here, we present a micro-total envelope system (mu-TES) and an automated total process for the generation of the carcinogenic reagent, its purification and its utilization for a desired synthesis that is totally enveloped from being exposed to the carcinogen. A unique microseparator is developed on the basis of SiNWs structure to replace the usual exposure-prone distillation in separating the generated reagent. Chloromethyl methyl ether chemistry is explored as a carcinogenic model in demonstrating the efficiency of the mu-TES that is fully automated so that feeding the ingredients for the generation is all it takes to produce the desired product. Syntheses taking days can be accomplished safely in minutes with excellent yields, which bodes well for elevating the carcinogenic chemistry to new unexplored dimensions.119Ysciescopu

    Highly photoresponsive and wavelength-selective circularly-polarized-light detector based on metal-oxides hetero-chiral thin film

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    A highly efficient circularly-polarized-light detector with excellent wavelength selectivity is demonstrated with an elegant and simple microelectronics-compatible way. The circularly-polarized-light detector based on a proper combination of the geometry-controlled TiO2-SnO2 hetero-chiral thin film as an effective chiroptical filter and the Si active layer shows excellent chiroptical response with external quantum efficiency as high as 30% and high helicity selectivity of similar to 15.8% in an intended wavelength range. Furthermore, we demonstrated the ability of manipulating both bandwidth and responsivity of the detector simultaneously in whole visible wavelength range by a precise control over the geometry and materials constituting hetero-chiral thin film. The high efficiency, wavelength selectivity and compatibility with conventional microelectronics processes enabled by the proposed device can result in remarkable developments in highly integrated photonic platforms utilizing chiroptical responses.1166Ysciescopu

    Massive type IIA string theory cannot be strongly coupled

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    Understanding the strong coupling limit of massive type IIA string theory is a longstanding problem. We argue that perhaps this problem does not exist; namely, there may be no strongly coupled solutions of the massive theory. We show explicitly that massive type IIA string theory can never be strongly coupled in a weakly curved region of space-time. We illustrate our general claim with two classes of massive solutions in AdS4xCP3: one, previously known, with N = 1 supersymmetry, and a new one with N = 2 supersymmetry. Both solutions are dual to d = 3 Chern-Simons-matter theories. In both these massive examples, as the rank N of the gauge group is increased, the dilaton initially increases in the same way as in the corresponding massless case; before it can reach the M-theory regime, however, it enters a second regime, in which the dilaton decreases even as N increases. In the N = 2 case, we find supersymmetry-preserving gauge-invariant monopole operators whose mass is independent of N. This predicts the existence of branes which stay light even when the dilaton decreases. We show that, on the gravity side, these states originate from D2-D0 bound states wrapping the vanishing two-cycle of a conifold singularity that develops at large N.Comment: 43 pages, 5 figures. v2: added reference

    A novel isolator-based system promotes viability of human embryos during laboratory processing

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    In vitro fertilisation (IVF) and related technologies are arguably the most challenging of all cell culture applications. The starting material is a single cell from which one aims to produce an embryo capable of establishing a pregnancy eventually leading to a live birth. Laboratory processing during IVF treatment requires open manipulations of gametes and embryos, which typically involves exposure to ambient conditions. To reduce the risk of cellular stress, we have developed a totally enclosed system of interlinked isolator-based workstations designed to maintain oocytes and embryos in a physiological environment throughout the IVF process. Comparison of clinical and laboratory data before and after the introduction of the new system revealed that significantly more embryos developed to the blastocyst stage in the enclosed isolator-based system compared with conventional open-fronted laminar flow hoods. Moreover, blastocysts produced in the isolator-based system contained significantly more cells and their development was accelerated. Consistent with this, the introduction of the enclosed system was accompanied by a significant increase in the clinical pregnancy rate and in the proportion of embryos implanting following transfer to the uterus. The data indicate that protection from ambient conditions promotes improved development of human embryos. Importantly, we found that it was entirely feasible to conduct all IVF-related procedures in the isolator-based workstations

    RepSeq-A database of amino acid repeats present in lower eukaryotic pathogens

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    BACKGROUND Amino acid repeat-containing proteins have a broad range of functions and their identification is of relevance to many experimental biologists. In human-infective protozoan parasites (such as the Kinetoplastid and Plasmodium species), they are implicated in immune evasion and have been shown to influence virulence and pathogenicity. RepSeq http://repseq.gugbe.com is a new database of amino acid repeat-containing proteins found in lower eukaryotic pathogens. The RepSeq database is accessed via a web-based application which also provides links to related online tools and databases for further analyses. RESULTS The RepSeq algorithm typically identifies more than 98% of repeat-containing proteins and is capable of identifying both perfect and mismatch repeats. The proportion of proteins that contain repeat elements varies greatly between different families and even species (3 - 35% of the total protein content). The most common motif type is the Sequence Repeat Region (SRR) - a repeated motif containing multiple different amino acid types. Proteins containing Single Amino Acid Repeats (SAARs) and Di-Peptide Repeats (DPRs) typically account for 0.5 - 1.0% of the total protein number. Notable exceptions are P. falciparum and D. discoideum, in which 33.67% and 34.28% respectively of the predicted proteomes consist of repeat-containing proteins. These numbers are due to large insertions of low complexity single and multi-codon repeat regions. CONCLUSION The RepSeq database provides a repository for repeat-containing proteins found in parasitic protozoa. The database allows for both individual and cross-species proteome analyses and also allows users to upload sequences of interest for analysis by the RepSeq algorithm. Identification of repeat-containing proteins provides researchers with a defined subset of proteins which can be analysed by expression profiling and functional characterisation, thereby facilitating study of pathogenicity and virulence factors in the parasitic protozoa. While primarily designed for kinetoplastid work, the RepSeq algorithm and database retain full functionality when used to analyse other species
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