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21.
Dipl.‐Chem. Alexander Zhdanko Dr. Markus Ströbele Prof. Dr. Martin E. Maier 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(46):14732-14744
Coordination chemistry of gold catalysts bearing eight different ligands [L=PPh3, JohnPhos (L2), Xphos (L3), DTBP, IMes, IPr, dppf, S‐tolBINAP (L8)] has been studied by NMR spectroscopy in solution at room temperature. Cationic or neutral mononuclear complexes LAuX (L=L2, L3, IMes, IPr; X=charged or neutral ligand) underwent simple ligand exchange without giving any higher coordinate complexes. For L2AuX the following ligand strength series was determined: MeOH?hex‐3‐yne <MeCN≈OTf??Me2S<2,6‐lutidine<4‐picoline<CF3CO2?≈DMAP<TMTU<PPh3<OH?≈Cl?. Some heteroligand complexes DTBPAuX exist in solution in equilibrium with the corresponding symmetrical species. Binuclear complexes dppf(AuOTf)2 and S‐tolBINAP(AuOTf)2 showed different behavior in exchange reactions with ligands depending on the ligand strength. Thus, PPh3 causes abstraction of one gold atom to give mononuclear complexes LLAuPPh3+ and (Ph3P)nAu+, but other N and S ligands give ordinary dicationic species LL(AuNu)22+. In reactions with different bases, LAu+ provided new oxonium ions whose chemistry was also studied: (DTBPAu)3O+, (L2Au)2OH+, (L2Au)3O+, (L3Au)2OH+, and (IMesAu)2OH+. Ultimately, formation of gold hydroxide LAuOH (L=L2, L3, IMes) was studied. Ligand‐ or base‐assisted interconversions between (L2Au)2OH+, (L2Au)3O+, and L2AuOH are described. Reactions of dppf(AuOTf)2 and S‐tolBINAP(AuOTf)2 with bases provided more interesting oxonium ions, whose molecular composition was found to be [dppf(Au)2]3O22+, L8(Au)2OH+, and [L8(Au)2]3O22+, but their exact structure was not established. Several reactions between different oxonium species were conducted to observe mixed heteroligand oxonium species. Reaction of L2AuNCMe+ with S2? was studied; several new complexes with sulfide are described. For many reversible reactions the corresponding equilibrium constants were determined. 相似文献
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The present study deals with the formulation of minimal loading conditions for microscale applications in numerical two-scale modelling (FE2) approaches. From the homogenisation concept, a set of volume average rules constrains the microscale PDE to be solved. They are considered to be the minimal set of loading conditions and can be specified by additional polynomial or periodic assumptions, for example, on the microscale displacement field. Whereas the resulting volume integrals can be transformed into surface integrals for so-called first-order homogenisation schemes, this is not possible for a second-order homogenisation of second gradient or micromorphic effective media substituting a heterogeneous microcontinuum represented by a volume element on the microscale. Several numerical examples compare the minimal loading condition concept with standard techniques discussed in literature. 相似文献
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Metal sheet forming processes like deep drawing are applied in order to produce carriage parts in mass production. Therefore, forming tools are required that are well protected against wear. For such forming tools, wear resistant surfaces are, e.g., produced by thermal spraying of hard material coatings. The thermal spraying process itself is a highly transient thermo-mechanical process. In order to gain a better understanding of the heat input and transfer during thermal spraying, a simulation framework for thermal spraying processes is presented. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
26.
Jiawang Liu Carolin Schneider Ji Yang Zhihong Wei Haijun Jiao Robert Franke Ralf Jackstell Matthias Beller 《Angewandte Chemie (International ed. in English)》2021,60(1):371-379
A chemo‐, regio‐, and stereoselective mono‐hydroamidation of (un)symmetrical 1,3‐diynes is described. Key for the success of this novel transformation is the utilization of an advanced palladium catalyst system with the specific ligand Neolephos. The synthetic value of this general approach to synthetically useful α‐alkynyl‐α, β‐unsaturated amides is showcased by diversification of several structurally complex molecules and marketed drugs. Control experiments and density‐functional theory (M06L‐SMD) computations also suggest the crucial role of the substrate in controlling the regioselectivity of unsymmetrical 1,3‐diynes. 相似文献
27.
Ralf Seemann Jean-Baptiste Fleury Corinna C. Maass 《The European physical journal. Special topics》2016,225(11-12):2227-2240
Self-propelled droplets are a special kind of self-propelled matter that are easily fabricated by standard microfluidic tools and locomote for a certain time without external sources of energy. The typical driving mechanism is a Marangoni flow due to gradients in the interfacial energy on the droplet interface. In this article we review the hydrodynamic prerequisites for self-sustained locomotion and present two examples to realize those conditions for emulsion droplets, i.e. droplets stabilized by a surfactant layer in a surrounding immiscible liquid. One possibility to achieve self-propelled motion relies on chemical reactions affecting the surface active properties of the surfactant molecules. The other relies on micellar solubilization of the droplet phase into the surrounding liquid phase. Remarkable cruising ranges can be achieved in both cases and the relative insensitivity to their own ‘exhausts’ allows to additionally study collective phenomena. 相似文献
28.
We address the quantum transition of a spin-1/2 antiferromagnetic Kondo lattice model with an easy-axis anisotropy using the extended dynamical mean field theory. We derive results in real frequency by using the bosonic numerical renormalization group (BNRG) method and compare them with quantum Monte Carlo results in Matsubara frequency. The BNRG results show a logarithmic divergence in the critical local spin susceptibility, signaling a destruction of Kondo screening. The T=0 transition is consistent with being second order. The BNRG results also display some subtle features; we identify their origin and suggest means for further microscopic studies. 相似文献
29.
Influence of higher harmonics of the undulator in X‐ray polarimetry and crystal monochromator design 下载免费PDF全文
Berit Marx‐Glowna Kai S. Schulze Ingo Uschmann Tino Kämpfer Günter Weber Christoph Hahn Hans‐Christian Wille Kai Schlage Ralf Röhlsberger Eckhart Förster Thomas Stöhlker Gerhard G. Paulus 《Journal of synchrotron radiation》2015,22(5):1151-1154
The spectrum of the undulator radiation of beamline P01 at Petra III has been measured after passing a multiple reflection channel‐cut polarimeter. Odd and even harmonics up to the 15th order, as well as Compton peaks which were produced by the high harmonics in the spectrum, could been measured. These additional contributions can have a tremendous influence on the performance of the polarimeter and have to be taken into account for further polarimeter designs. 相似文献
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