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Dr. Massimo Rigo Evi R. M. Habraken Dr. Koyel Bhattacharyya Manuela Weber Dr. Andreas W. Ehlers Dr. Nicolas Mézailles Dr. J. Chris Slootweg Prof. Dr. Christian Müller 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(37):8769-8779
A series of substituted phosphinines, 1-phosphabarrelenes and 5-phosphasemibullvalenes were synthesized and evaluated for their potential application as ligands in homogeneous catalytic reactions. While their buried volume (%Vbur) was calculated to get insight into the steric properties, [LNi(CO)3] complexes were prepared in order to determine the corresponding Tolman electronic parameter. ETS-NOCV (extended-transition-state natural orbital for chemical valence) calculations on [LAuCl] complexes further allowed an estimation of the σ- and π-contributions to the L− M interaction. AuI coordination compounds of selected examples were prepared and characterized by single crystal X-ray diffraction. Finally, the three classes of PIII compounds were successfully used in the AuI-catalyzed cycloisomerization of N-2-propyn-1-ylbenzamide, showing very good activities and selectivities, which are comparable with the reported data of cationic phosphorus-based gold catalysts. 相似文献
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The test of the validity of the Fromhold-Cook theory of metal oxidation for the O2/Fe system in the tunnel regime is impeded by the growth of a passivating Fe2+/Fe3+ double layer at T=150 degrees C. However, during an intermediate anneal step at 200 degrees C, the Fe3+ is reduced to Fe2+. The oxidation rate of this annealed layer is in agreement with the Fromhold-Cook theory. At room temperature, the ionic current is rate limiting. For T>150 degrees C, the thermionic emission of electrons is rate limiting for oxygen coverages larger than 13x10(15) atoms/cm(2). 相似文献
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P. Flores L. Duchêne C. Bouffioux T. Lelotte C. Henrard N. Pernin A. Van Bael S. He J. Duflou A.M. Habraken 《International Journal of Plasticity》2007
The bi-axial experimental equipment [Flores, P., Rondia, E., Habraken, A.M., 2005a. Development of an experimental equipment for the identification of constitutive laws (Special Issue). International Journal of Forming Processes] developed by Flores enables to perform Bauschinger shear tests and successive or simultaneous simple shear tests and plane strain tests. Flores investigates the material behavior with the help of classical tensile tests and the ones performed in his bi-axial machine in order to identify the yield locus and the hardening model. With tests performed on one steel grade, the methods applied to identify classical yield surfaces such as [Hill, R., 1948. A theory of the yielding and plastic flow of anisotropic materials. Proceedings of the Royal Society of London A 193, 281–297; Hosford, W.F., 1979. On yield loci of anisotropic cubic metals. In: Proceedings of the 7th North American Metalworking Conf. (NMRC), SME, Dearborn, MI, pp. 191–197] ones as well as isotropic Swift type hardening, kinematic Armstrong–Frederick or Teodosiu and Hu hardening models are explained. Comparison with the Taylor–Bishop–Hill yield locus is also provided. The effect of both yield locus and hardening model choices is presented for two applications: plane strain tensile test and Single Point Incremental Forming (SPIF). 相似文献
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Rutger J. I. Knoop Gijs J. M. Habraken Nicolas Gogibus Simone Steig Henning Menzel Cor E. Koning Andreas Heise 《Journal of polymer science. Part A, Polymer chemistry》2008,46(9):3068-3077
We have developed a metal free synthetic pathway to homopolypeptide rod‐coil block copolymers. The concept was proven for the synthesis of poly(benzyl‐L ‐glutamate‐b‐styrene). A dual initiator containing a primary amine and a nitroxide group was used in a macroinitiation approach with high initiation efficiency. Good control over the molecular weight in the ring opening polymerization of benzyl‐L ‐glutamate N‐carboxyanhydride was obtained in DMF at 0 °C yielding poly(benzyl‐L ‐glutamates) with low polydispersities around 1.1. The almost quantitative incorporation of the dual initiator was confirmed by MALDI‐ToF analysis. Macroinitiation of styrene by nitroxide‐mediated controlled radical polymerization yielded the block copolymer with high structural control. The diblock structure was confirmed by molecular weight increase upon macroinitiation by size exclusion chromatography and retention time comparison with homopolymers using gradient polymer elution chromatography. Both polymerizations were also successfully conducted in one pot without intermediate isolation owing to the high compatibility of both polymerization techniques. © 2008 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 46: 3068–3077, 2008 相似文献
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We study geometric phases that arise from (cyclic) transformations of the transverse spatial structure of paraxial optical modes. Our approach involves bosonic ladder operators that, in the spirit of the quantum-mechanical harmonic oscillator, generate sets of transverse optical modes. It applies to modes of all orders in a very natural way and provides a universal geometric interpretation of the phase shifts acquired by nonastigmatic modes under typical experimental conditions. 相似文献
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Julia Leitl Dr. Andrew R. Jupp Dr. Evi R. M. Habraken Verena Streitferdt Dr. Peter Coburger Dr. Daniel J. Scott Prof. Dr. Ruth M. Gschwind Prof. Dr. Christian Müller Dr. J. Chris Slootweg Prof. Dr. Robert Wolf 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(35):7788-7800
Salt metathesis of 1-methyl-2,4,6-triphenylphosphacyclohexadienyl lithium and chlorobis(pentafluorophenyl)borane affords a 1-phospha-7-bora-norbornadiene derivative 2 . The C≡N triple bonds of nitriles insert into the P−B bond of 2 with concomitant C−B bond cleavage, whereas the C≡C bonds of phenylacetylenes react with 2 to form λ4-phosphabarrelenes. Even though 2 must formally be regarded as a classical Lewis adduct, the C≡N and C≡C activation processes observed (and the mild conditions under which they occur) are reminiscent of the reactivity of frustrated Lewis pairs. Indeed, NMR and computational studies give insight into the mechanism of the reactions and reveal the labile nature of the phosphorus–boron bond in 2 , which is also suggested by detailed NMR spectroscopic studies on this compound. Nitrile insertion is thus preceded by ring opening of the bicycle of 2 through P−B bond splitting with a low energy barrier. By contrast, the reaction with alkynes involves formation of a reactive zwitterionic methylphosphininium borate intermediate, which readily undergoes alkyne 1,4-addition. 相似文献
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Simone Steig Frauke Cornelius Andreas Heise Rutger J. I. Knoop Gijs J. M. Habraken Cor E. Koning Henning Menzel 《Macromolecular Symposia》2007,248(1):199-206
A double-headed initiator was synthesized yielding two functional groups for the initiation of the nickel mediated ring-opening polymerization of γ-benzyl-L -glutamate-N-carboxyanhydride and controlled radical polymerization of vinyl monomers via ATRP or NMP. Well-defined block copolymers combining polypeptides and synthetic polymers were obtained. 相似文献