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761.
In Francfort and Marigo's variational free-discontinuity formulation of brittle fracture [1] cracking is regarded as an energy minimization process, where the total energy is minimized with respect to any admissible crack set and displacement field. No additional criterion is needed to determine crack paths, branching of cracks and crack initiations. However, a direct discretization of the model is faced with significant technical problems, as it involves minimizations in a set of possibly discontinuous functions. A regularized version of the model has been introduced by Bourdin [2] and based on this, we use the concept of a continuum phase field model to simulate cracking processes. Cracks are indicated by the order parameter of the phase field model and cracking can be regarded as a phase transition problem. Additionally, introducing the heat equation into the model, it is capable to also take account of crack propagation due to thermal stresses. In the numerical implementation, crack parameter as well as temperature are treated as additional degrees of freedom and the coupled field equations are solved using the finite element method together with an implicit time integration scheme. (© 2009 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
762.
James J. Race Alex Heyam Matthew A. Wiebe J. Diego-Garcia Hernandez Charlotte E. Ellis Shixing Lei Ian Manners Andrew S. Weller 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(3):e202216106
An amphiphilic block copolymer of polyphosphinoborane has been prepared by a mechanism-led strategy of the sequential catalytic dehydropolymerization of precursor monomers, H3B ⋅ PRH2 (R=Ph, n-hexyl), using the simple pre-catalyst [Rh(Ph2PCH2CH2PPh2)2]Cl. Speciation, mechanism and polymer chain growth studies support a step-growth process where reversible chain transfer occurs, i.e. H3B ⋅ PRH2/oligomer/polymer can all coordinate with, and be activated by, the catalyst. Block copolymer [H2BPPhH]110-b-[H2BP(n-hexyl)H]11 can be synthesized and self-assembles in solution to form either rod-like micelles or vesicles depending on solvent polarity. 相似文献
763.
Charlotte Hampton Dr. Marco Simonetti Prof. Daniele Leonori 《Angewandte Chemie (International ed. in English)》2023,62(8):e202214508
Vicinal diols are abundant among natural and synthetic molecules, and also represent valuable intermediates throughout organic synthesis. Olefin dihydroxylation is an effective strategy to access these derivatives owing to the broad range and availability of alkene feedstocks. OsO4 is among the most used reagents to achieve this transformation, yet its high toxicity and cost remain concerning. Herein, we present a mechanistically distinct strategy for olefin dihydroxylation using nitroarenes as photoresponsive oxidants. Upon purple LEDs irradiation, these species undergo a [3+2]-photocycloaddition with a wide range of olefins to give stable 1,3,2-dioxazolidine intermediates. These species can be accumulated in solution and then reduced in situ to the desired diols, utilising readily accessible and easy to handle solid reagents as H2 surrogates. 相似文献
764.
765.
Davide Derelli Francesco Caddeo Kilian Frank Kilian Krötzsch Patrick Ewerhardt Marco Krüger Sophie Medicus Lars Klemeyer Marvin Skiba Charlotte Ruhmlieb Olof Gutowski Ann-Christin Dippel Wolfgang J. Parak Bert Nickel Dorota Koziej 《Angewandte Chemie (International ed. in English)》2023,62(43):e202307948
CuBi2O4 has recently emerged as a promising photocathode for photo-electrochemical (PEC) water splitting. However, its fast degradation under operation currently poses a limit to its application. Here, we report a novel method to study operando the semiconductor-electrolyte interface during PEC operation by surface-sensitive high-energy X-ray scattering. We find that a fast decrease in the generated photocurrents correlates directly with the formation of a metallic Bi phase. We further show that the slower formation of metallic Cu, as well as the dissolution of the electrode in contact with the electrolyte, further affect the CuBi2O4 activity and morphology. Our study provides a comprehensive picture of the degradation mechanisms affecting CuBi2O4 electrodes under operation and poses the methodological basis to investigate the photocorrosion processes affecting a wide range of PEC materials. 相似文献
766.
767.
Charlotte M. Wentz Kätchen K. Lachmayr Dr. Esther H. R. Tsai Prof. Dr. Lawrence R. Sita 《Angewandte Chemie (International ed. in English)》2023,62(23):e202302739
Experimental results are presented that serve to lower the barrier for developing the science and technology of non-classical thermotropic glycolipid mesophases, which now include dodecagonal quasicrystal (DDQC) and Frank–Kasper (FK) A15 and σ mesophases that can be produced under mild conditions from a versatile class of sugar-polyolefin conjugates. By employing “alloys” comprised of mono- and disaccharide-polyolefin conjugates, and optionally with vitamin E as a small molecule phase modulator, we report the spontaneous formation of stable A15 mesophases at ambient temperature. We further document a rich thermotropic phase map that includes DDQC, A15, and σ mesophases of tunable periodicity that are connected through rapid thermotropic phase transitions as a function of increasing temperature in the order: liquid-like packing (LLP)→DDQC → A15→σ→ disorder. This first direct observation of a rapid thermotropic A15→σ phase transition provides support for a diffusionless martensitic process proceeding through strain-induced introduction of planar defects into the A15 lattice. 相似文献