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101.
Asymmetric Hydroalkoxylation of Non‐Activated Alkenes: Titanium‐Catalyzed Cycloisomerization of Allylphenols at High Temperatures
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M. Sc. Johannes Schlüter M. Sc. Max Blazejak Dr. Florian Boeck Prof. Dr. Lukas Hintermann 《Angewandte Chemie (International ed. in English)》2015,54(13):4014-4017
The asymmetric catalytic addition of alcohols (phenols) to non‐activated alkenes has been realized through the cycloisomerization of 2‐allylphenols to 2‐methyl‐2,3‐dihydrobenzofurans (2‐methylcoumarans). The reaction was catalyzed by a chiral titanium–carboxylate complex at uncommonly high temperatures for asymmetric catalytic reactions. The catalyst was generated by mixing titanium isopropoxide, the chiral ligand (aS)‐1‐(2‐methoxy‐1‐naphthyl)‐2‐naphthoic acid or its derivatives, and a co‐catalytic amount of water in a ratio of 1:1:1 (5 mol % each). This homogeneous thermal catalysis (HOT‐CAT) gave various (S)‐2‐methylcoumarans with yields of up to 90 % and in up to 85 % ee at 240 °C, and in 87 % ee at 220 °C. 相似文献
102.
Porous and Shape‐Anisotropic Single Crystals of the Semiconductor Perovskite CH3NH3PbI3 from a Single‐Source Precursor
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Tom Kollek Dominik Gruber Julia Gehring Eugen Zimmermann Prof. Dr. Lukas Schmidt‐Mende Prof. Dr. Sebastian Polarz 《Angewandte Chemie (International ed. in English)》2015,54(4):1341-1346
Significant progress in solar‐cell research is currently made by the development of metal–organic perovskites (MOPs) owing to their superior properties, such as high absorption coefficients and effective transport of photogenerated charges. As for other semiconductors, it is expected that the properties of MOPs may be significantly improved by a defined nanostructure. However, their chemical sensitivity (e.g., towards hydrolysis) prohibits the application of methods already known for the synthesis of other nanomaterials. A new and general method for the synthesis of various (CH3NH3)PbI3 nanostructures from a novel single‐source precursor is presented. Nanoporous MOP single crystals are obtained by a crystal‐to‐crystal transformation that is accompanied by spinodal demixing of the triethylene glycol containing precursor structure. Selective binding of a capping agent can be used to tune the particle shape of the MOP nanocrystals. 相似文献
103.
Jiri Kudr Sylvie Skalickova Lukas Nejdl Amitava Moulick Branislav Ruttkay–Nedecky Vojtech Adam Rene Kizek 《Electrophoresis》2015,36(19):2367-2379
Nanofluidics is becoming an extensively developing technique in the field of bioanalytical chemistry. Nanoscale hole embed in an insulating membrane is employed in a vast variety of sensing platforms and applications. Although, biological nanopores have several attractive characteristics, in this paper, we focused on the solid‐state nanopores due to their advantages as high stability, possibility of diameter control, and ease of surface functionalizing. A detection method, based on the translocation of analyzed molecules through nanochannels under applied voltage bias and resistive pulse sensing, is well established. Nevertheless, it seems that the new detection methods like measuring of transverse electron tunneling using nanogap electrodes or optical detection can offer significant additional advantages. The aim of this review is not to cite all related articles, but highlight the steps, which in our opinion, meant important progresses in solid‐state nanopore analysis. 相似文献
104.
Lukas Stolzer Antonina Vigovskaya Prof. Christopher Barner‐Kowollik Dr. Ljiljana Fruk 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(41):14309-14313
A photochemical approach based on nitrile imine‐mediated tetrazole‐ene cycloaddition is introduced to functionalize gold nanorods with biomolecules. For this purpose, a bifunctional, photoreactive linker containing thioctic acid as the Au anchoring group and a tetrazole moiety for the light‐induced reaction with maleimide‐capped DNA was prepared. The tetrazole‐based reaction on the nanoparticles’ surface results in a fluorescent pyrazoline product allowing for the spectroscopic monitoring of the reaction. This first example of nitrile imine‐mediated tetrazole‐ene cycloaddition (NITEC)‐mediated biofunctionalization of Au nanorods paves the way for the attachment of sensitive biomolecules, such as antibodies and other proteins, under mild conditions and expands the toolbox for the tailoring of nanomaterials. 相似文献
105.
Very Facile Polarity Umpolung and Noncovalent Functionalization of Inorganic Nanoparticles: A Tool Kit for Supramolecular Materials Chemistry
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Lukas Zeininger Stefanie Petzi Jörg Schönamsgruber Luis Portilla Prof. Dr. Marcus Halik Prof. Dr. Andreas Hirsch 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(40):14030-14035
The facile assembly of shell‐by‐shell (SbS)‐coated nanoparticles [TiO2?PAC16]@shell 1 – 7 (PAC16=hexadecylphosphonic acid), which are soluble in water and can be isolated as stable solids, is reported. In these functional architectures, an umpolung of dispersibility (organic apolar versus water) was accomplished by the noncovalent binding of ligands 1 – 7 to titania nanoparticles [TiO2?PAC16] containing a first covalent coating with PAC16. Ligands 1 – 7 are amphiphilic and form the outer second shell of [TiO2?PAC16]@shell 1 – 7 . The tailor‐designed dendritic building blocks 3 – 5 contain negative and positive charges in the same molecule, and ligands 6 and 7 contain a perylenetetracarboxylic acid dimide (PDI) core ( 6 / 7 ) as a photoactive reporter component. In the redox and photoactive system [TiO2?PAC16]@shell 7 , electronic communication between the inorganic core to the PDI ligands was observed. 相似文献
106.
The characteristics of a manufacturing product are influenced by a variety of different factors, such as the material properties of the base product. The prediction of properties that give optimal results in metal forming applications is a complex task but of high interest for the manufacturer. To realize such a prediction scheme, the process chain is split up into individual process steps and for each of them an inverse modeling is required. The specific aim of this work is to present an approach for the inverse problem formulation of a process step and to solve it using methods of machine learning. Moreover, the challenges that often arise due to the ill-posed nature of inverse problems will be discussed. The main focus is on the crystallographic texture of metals, which strongly affects the deformation behavior during a process step and highly influences the characteristics of the final product. (© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
107.
In this short note, we give a characterization of domains satisfying Serre’s condition (R1) in terms of their canonical modules. In the special case of toric rings, this generalizes a result of the second author [9] where the normality is described in terms of the “shape” of the canonical module. 相似文献
108.
Susan Torabi Lukas Hammerschmidt Elena Voloshina Beate Paulus 《International journal of quantum chemistry》2014,114(14):943-951
The performance of wavefunction‐based correlation methods in theoretical solid‐state chemistry depends on reliable Hartree–Fock (HF) results for infinitly extended systems. Therefore, we optimized basis sets of valence‐triple‐ζ quality based on HF calculations for the periodic system of group‐12‐metal difluorides. Scalar‐relativistic effects were included in the case of the metal‐ions by applying small‐core pseudopotentials. To assess the quality of the proposed basis sets, the structural parameters, bulk moduli as well as cohesive and lattice energies of the systems were evaluated at the HF and the density functional theory levels. In addition to these two mean‐field approaches and to assess further employment of our basis sets to wavefunction‐based correlation methods we performed periodic local MP2 computations. Finally, the possibilities of pressure induced structural phase transitions occurring in the ZnF2, CdF2, and HgF2 were investigated. © 2014 Wiley Periodicals, Inc. 相似文献
109.
Structural stability is an important issue to ensure the safety of thin walled structures. Shell structures are considered in context of linear and non-linear buckling. The design sensitivity analysis with respect to modifications in shape is motivated. Analytically derived gradient information is employed for shape optimisation purposes using solid shells. (© 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
110.