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151.
Dr. Christine Dietrich Si Chen Georgios Uzunidis Dr. Martin Hähsler Yannick Träutlein Dr. Silke Behrens 《ChemistryOpen》2021,10(2):296-304
Multimetallic nanoparticles often enhance the catalytic performance of their monometallic counterparts by increasing reaction rates, catalyst selectivity, and/or stability. A prerequisite for understanding structure- and composition-associated properties, however, is the careful design of multimetallic nanoparticles with various structures and compositions. Here, bimetallic Pd/Sn-based nanoparticles are prepared with a tunable composition and structure exploiting ionic liquids (ILs) as reaction medium (i. e., methyltrioctylammonium bis(trifluoromethylsulfonyl)imide). The nanoparticles are obtained in a one-pot synthetic procedure by reducing the metal salt precursors with triethylborohydride in the IL. The results show that the reaction parameters, in particular the nature and ratio of the Pd2+/Sn2+ precursors as well as the reaction temperature, influence NP formation and composition. X-ray diffraction with Rietveld analysis and transmission electron microscopy are employed to determine NP size and phase composition. Under optimized reaction conditions Pd2Sn or PdSn nanocrystals are formed as single-phase products after introducing an additional annealing step at 200 °C. Nanocrystals with intermetallic composition reveal enhanced catalytic properties in the semihydrogenation of diphenylacetylene which was used as a model reaction. 相似文献
152.
We establish a generalization of Breen's theory of cubic structures on line bundles over group schemes. We study such “n-cubic structures” inductively using multiextensions. As a result we obtain information on the set of isomorphism classes of line bundles with n-cubic structures over finite multiplicative group schemes over Spec(Z) by relating this set to certain corresponding eigenspaces of ideal class groups of cyclotomic fields. 相似文献
153.
We give, using an explicit expression obtained in (Jones V, Ann Math 126:335, 1987), a basic hypergeometric representation of the HOMFLY polynomial of (n, m) torus knots, and present a number of equivalent expressions, all related by Heine’s transformations. Using this result, the \({ (m, n) \leftrightarrow (n, m)}\) symmetry and the leading polynomial at large N are explicit. We show the latter to be the Wilson loop of 2d Yang–Mills theory on the plane. In addition, after taking one winding to infinity, it becomes the Wilson loop in the zero instanton sector of the 2d Yang–Mills theory, which is known to give averages of Wilson loops in \({\mathcal{N}}\) = 4 SYM theory. We also give, using matrix models, an interpretation of the HOMFLY polynomial and the corresponding Jones–Rosso representation in terms of q-harmonic oscillators. 相似文献
154.
155.
We describe an efficient generalized Born (GB) approximation for proteins, in which the interaction energy between two amino acids depends on the whole protein structure, but can be accurately computed from residue-pairwise information. Two results make the scheme pairwise. First, an accurate expression exists for the interaction energy between two residues R and R' that depends on the product B = BRBR' of their residue Born solvation radii. Second, this expression is accurately fitted by a parabolic function of B; the (three) fitting coefficients depend only on the pair RR', not on its environment. In effect, the quantity B captures all the information that is relevant about the pair's dielectric environment. The method is tested with calculations on several hundred structures of the proteins trpcage, BPTI, ubiqutin, and thoredoxin. It yields solvation energies in better agreement with Poisson calculations than a traditional GB formulation. We also compute the effect of the protein/solvent environment on the interactions between pairs of charged residues in the active site of the enzyme aspartyl-tRNA synthetase. Our method captures this effect as accurately as traditional GB. Because it is residue-pairwise, the method can be incorporated into efficient protocols for rotamer placement and computational protein design. 相似文献
156.
Andreas Grenner Georgios M. KontogeorgisNicolas von Solms Michael L. Michelsen 《Fluid Phase Equilibria》2007
The simplified PC-SAFT equation of state has been applied to liquid–liquid, vapor–liquid and solid–liquid equilibria for mixtures containing 1- or 2-alkanols with alkanes, aromatic hydrocarbons, CO2 and water. For the alkanols we use generalized pure compound parameters. This means that two of the physical pure compound parameters, m (segment number) and σ (segment diameter), are obtained from linear extrapolations, since m and mσ3, increase linearly with respect to the molar mass, and moreover, the two association parameters (association energy and association volume) were assumed to be constant for all alkanols. Only the dispersion energy is fitted to experimental data. Thus it is possible to estimate parameters for several 1- and 2-alkanols. The final aim is to develop a group contribution approach for PC-SAFT which is suitable for complex compounds, considering that the motivation of this project is to obtain a thermodynamic model which can be used in the development of sophisticated products such as pharmaceuticals, polymers, detergents or food ingredients. One of the severe limitations in applying SAFT-type equations of state to these compounds is that the procedure for obtaining the pure compound parameters is usually based on fitting to saturated vapor pressure and liquid density data over an extended temperature range. However, such data are rarely available for complex compounds. To verify the new pure compound parameters, comparisons to ordinary optimized alkanol parameters, where all five pure compound parameters were fitted to experimental liquid density and vapor pressure data, were made. The results show that the new generalized alkanol parameters from this work perform at least as well as other alkanol parameter sets. 相似文献
157.
Ioannis D. Kostas Athanassios G. Coutsolelos Georgios Charalambidis 《Tetrahedron letters》2007,48(38):6688-6691
For the first time, a palladium complex with a porphyrin ligand is used as a catalyst precursor for cross-coupling reactions. The synthesis of a palladium complex with a phosphine-free and water-soluble potassium carboxylate salt of a porphyrin, and its evaluation in the Suzuki-Miyaura reaction of phenylboronic acid with aryl bromides (from electron-rich to electron-poor), in neat water, under aerobic conditions is described. Catalysis is performed at 100 °C for 4 h, using K2CO3 as base, and a substrate to catalyst molar ratio of 1000:1, leading to yields of coupling products in the range of 80-100%. The catalyst can be recycled and reused, but unfortunately, with a loss in activity. 相似文献
158.
Ioannis Polyzos Georgios Tsigaridas Mihalis Fakis John Parthenios Anastassios Fragos Vassilis Giannetas Peter Persephonis John Mikroyannidis 《Monatshefte für Chemie / Chemical Monthly》2001,132(1):169-175
Summary. Two-photon absorption induced fluorescence microscopy was used as a tool for the examination of the spatial distribution
of a thin dye film. The two-photon absorption induced fluorescence signal is essentially the same as that produced by excitation
with a single photon of equivalent energy. When femtosecond pulses are focused into a sample there is an intrinsic spatial
selectivity of the two-photon emission signal, since it is dependent upon the square of the light intensity. This has tremendous
implications in fluorescence microscopy. Since two-photon absorption is confined in a small region at the focal waist of an
objective lens, photodamage and photobleaching of the sample are significantly reduced. In addition, the two-photon signal
has inherent z-axis spatial resolution, which facilitates the construction of 3-D images. In the present work an application of this technique
to a thin film of a dye is presented. The method can generally be applied to thin films made from photonic polymers.
Received June 23, 2000. Accepted (revised) July 31, 2000 相似文献
159.
Ataulla Shegiwal Alan M. Wemyss Mike A. J. Schellekens Jens de Bont James Town Evelina Liarou Georgios Patias Christophe J. Atkins David M. Haddleton 《Journal of polymer science. Part A, Polymer chemistry》2019,57(3):E1-E9
We present a systematic study of incorporating carboxyl groups into latex particles to enhance colloidal stability and the physical properties of the latex. Statistical copolymers of methacrylic acid and methyl methacrylate) were synthesized via catalytic chain transfer polymerization (CCTP) in emulsion. The vinyl‐terminated oligomers were in turn successfully utilized as chain transfer agents for the formation of diblock and pseudo triblock copolymers via sulfur‐free reversible addition–fragmentation chain transfer polymerization (SF‐RAFT). These copolymers were characterized using 1H NMR, size exclusion chromatography (SEC), dynamic light scattering (DLS), dynamic mechanical analysis (DMA), contact angle measurements and matrix‐assisted laser desorption/ionization time of flight mass spectroscopy (MALDI‐TOF‐MS) techniques. © 2019 The Authors. Journal of Polymer Science Part A: Polymer Chemistry published by Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019 , 57, E1–E9 相似文献
160.
Dr. Georgios Rotas Prof. Dr. Nikos Tagmatarchis 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(4):1206-1214
Energy conversion schemes have attracted considerable attention in recent years. A large amount of research effort has focused on fullerenes, particularly C60 and its derivatives, as suitable electron acceptors, owing to their outstanding properties. In this context, C59N‐based donor–acceptor systems have lately attracted attention, owing to their exceptional energy‐and electron‐transfer properties. As a result, chemical derivatization of C59N plays an important role in the realization of the aforementioned systems. The current Minireview aims to familiarize researchers with the main aspects of azafullerene synthesis, chemistry, and photophysical properties, while it mainly focuses on the synthetic methodologies employed for as well as on energy conversion schemes of azafullerene‐based donor–acceptor systems. 相似文献