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991.
Daniel Joven-Sancho Dr. Miguel Baya Prof. Dr. Larry R. Falvello Dr. Antonio Martín Dr. Jesús Orduna Dr. Babil Menjón 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(50):12796-12806
The involvement of silver in two-electron AgI/AgIII processes is currently emerging. However, the range of stability of the required and uncommon AgIII species is virtually unknown. Here, the stability of AgIII towards the whole set of halide ligands in the organosilver(III) complex frame [(CF3)3AgX]− (X=F, Cl, Br, I, At) is theoretically analyzed. The results obtained depend on a single factor: the nature of X. Even the softest and least electronegative halides (I and At) are found to form reasonably stable AgIII−X bonds. Our estimates were confirmed by experiment. The whole series of nonradiative halide complexes [PPh4][(CF3)3AgX] (X=F, Cl, Br, I) has been experimentally prepared and all its constituents have been isolated in pure form. The pseudohalides [PPh4][(CF3)3AgCN] and [PPh4][(CF3)3Ag(N3)] have also been isolated, the latter being the first silver(III) azido complex. Except for the iodo compound, all the crystal and molecular structures have been established by single-crystal X-ray diffraction methods. The decomposition paths of the [(CF3)3AgX]− entities at the unimolecular level have been examined in the gas phase by multistage mass spectrometry (MSn). The experimental detection of the two series of mixed complexes [CF3AgX]− and [FAgX]− arising from the corresponding parent species [(CF3)3AgX]− demonstrate that the Ag−X bond is particularly robust. Our experimental observations are rationalized with the aid of theoretical methods. Smooth variation with the electronegativity of X is also observed in the thermolyses of bulk samples. The thermal stability in the solid state gradually decreases from X=F (145 °C, dec.) to X=I (78 °C, dec.) The experimentally established compatibility of AgIII with the heaviest halides is of particular relevance to silver-mediated or silver-catalyzed processes. 相似文献
992.
Dr. Gabriele Hierlmeier Dr. Peter Coburger Dr. Daniel J. Scott Dr. Thomas M. Maier Dr. Stefan Pelties Prof. Dr. Robert Wolf Daniel M. Pividori Prof. Dr. Karsten Meyer Dr. Nicolaas P. van Leest Prof. Dr. Bas de Bruin 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(60):14936-14946
Reactions of di-tert-butyldiphosphatetrahedrane ( 1 ) with cycloocta-1,5-diene- or anthracene-stabilised metalate anions of iron and cobalt consistently afford complexes of the rarely encountered 1,2-diphosphacyclobutadiene ligand, which have previously been very challenging synthetic targets. The subsequent reactivity of 1,2-diphosphacyclobutadiene cobaltates toward various electrophiles has also been investigated and is compared to reactions of related 1,3-diphosphacyclobutadiene complexes. The results highlight the distinct reactivity of such isomeric species, showing that the 1,2-isomers can act as precursors for previously unknown triphospholium ligands. The electronic structures of the new complexes were investigated by several methods, including NMR, EPR and Mößbauer spectroscopies as well as quantum chemical calculations. 相似文献
993.
Kwan Ho Au-Yeung Tim Kühne Daniel Becker Dr. Marcus Richter Dr. Dmitry A. Ryndyk Prof. Dr. Gianaurelio Cuniberti Prof. Dr. Thomas Heine Prof. Dr. Xinliang Feng Dr. Francesca Moresco 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(69):17336-17340
The rapid development of on-surface synthesis provides a unique approach toward the formation of carbon-based nanostructures with designed properties. Herein, we present the on-surface formation of CN-substituted phenylene vinylene chains on the Au(111) surface, thermally induced by annealing the substrate stepwise at temperatures between 220 °C and 240 °C. The reaction is investigated by scanning tunneling microscopy and density functional theory. Supported by the calculated reaction pathway, we assign the observed chain formation to a Knoevenagel condensation between an aldehyde and a methylene nitrile substituent. 相似文献
994.
995.
Rui P. Queirós Daniel Rainho Mauro D. Santos Liliana G. Fidalgo Ivonne Delgadillo 《高压研究》2015,35(1):69-77
This study evaluated high pressure processing (P1 – 400?MPa/5?min; P2 – 550?MPa/2?min) and thermal pasteurization (TP – 70°C/30?s) effects on sweet cherry juice's microbiological and physicochemical parameters, during four weeks of refrigerated storage. All treatments reduced the microbiological load to undetectable levels not affecting total soluble solids and titratable acidity. The pH increased with all treatments, however, it decreased during storage. Phenols were differently affected: TP increased them by 6%, P1 had no effect while P2 decreased them by 11%. During storage, phenols in control and TP samples decreased by 26% and 20%, P1 samples decreased them by 11% whereas P2 showed no variation. TP had no effect on anthocyanins, while pressure treatments increased them by 8%. Anthocyanins decreased during storage, particularly in the control and P1 (decreasing 41%). All treatments had no effect on antioxidant activity until the 14th day, thereafter high pressure processing samples showed the highest antioxidant activity. 相似文献
996.
997.
Daniel Oron 《The Journal of the Operational Research Society》2015,66(5):732-736
In this paper, we consider a single machine no-wait scheduling model whereby job processing times are general functions of their position in the job sequence. We assume that the single machine must operate at a certain cycle, which can be determined by the scheduler. Furthermore, exactly one job has to be completed by the end of each cycle. Using different variations of the Linear Assignment Problem formulation, we develop polynomial time algorithms for minimizing the following objectives: makespan, total completion time, maximum earliness and total earliness. 相似文献
998.
A combined transient and steady state approach for robust lifetime spectroscopy with micrometer resolution
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We present the combination of two complementary micro‐photoluminescence spectroscopic techniques operating in transient and steady state condition, respectively. Introducing the time domain into the well‐established micro‐photoluminescence mapping approach operating under steady state conditions demonstrates a distinct improvement of the robustness and reliability in the determination of charge carrier lifetime measured with micrometer spatial resolution. Lifetimes from 50 ns to above ms are accessible. We elaborate a calibration procedure and apply the combined all‐photoluminescence setup to high‐performance multicrystalline silicon. A lifetime image obtained from the established photoluminescence imaging technique is reconstructed from the microscopic map by considering lateral diffusion and optical blurring, revealing a more detrimental influence of small angle grain boundaries as well as a higher lifetime within grains as may be deduced from the standard imaging technique. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim) 相似文献
999.
1000.