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81.
Ruben M Ziener U Lehn JM Ksenofontov V Gütlich P Vaughan GB 《Chemistry (Weinheim an der Bergstrasse, Germany)》2004,11(1):94-100
Hierarchical self-assembly of complex supramolecular architectures allows for the emergence of novel properties at each level of complexity. The reaction of the ligand components A and B with Fe(II) cations generates the [2x2] grid-type functional building modules 1 and 2, presenting spin-transition properties and preorganizing an array of coordination sites that sets the stage for a second assembly step. Indeed, binding of La(III) ions to 1 and of Ag(I) ions to 2 leads to a 1D columnar superstructure 3 and to a wall-like 2D layer 4, respectively, with concomitant modulation of the magnetic properties of 1 and 2. Thus, to each of the two levels of structural complexity generated by the two sequential self-assembly steps corresponds the emergence of novel functional features. 相似文献
82.
Barboiu M Cerneaux S van der Lee A Vaughan G 《Journal of the American Chemical Society》2004,126(11):3545-3550
We report new hybrid organic-inorganic materials, based on macrocyclic receptors 1-3 self-organized in tubular superstructures prepared by sol-gel process. Fourier transform infrared (FTIR) and NMR spectroscopic analyses demonstrate that the self-organization by hydrogen bonding of organogel superstructures of 2 and 3 were preserved in the hybrid materials throughout the sol-gel process. The molecular arrangement of heteroditopic receptors defines a particularly attractive functional transport device for both cation (tubular macrocycles) and anion (sandwich-urea) directional-diffusion transport mechanism in the hybrid membrane material. This system has been employed successfully to design a solid dense membrane, functioning as an ion-powered adenosine triphosphate (ATP(2)(-)) pump, and illustrates how a self-organized hybrid material performs interesting and potentially useful functions. 相似文献
83.
84.
Wan‐Ping Hu Vaughan S. Langford Murray J. McEwan Daniel B. Milligan Malina K. Storer Jack Dummer Michael J. Epton 《Rapid communications in mass spectrometry : RCM》2010,24(12):1744-1748
The selectivity and sensitivity of selected ion flow tube mass spectrometry (SIFT‐MS) for individual breath analysis of haloamines has been improved by heating the flow tube in a commercial instrument to around 106°C. Data is presented showing the marked reduction in the number density of water clusters of product ions of common breath metabolites that are isobaric with the product ions from monochloramine and monobromamine that are used to monitor the haloamine concentrations. These results have direct relevance to the real‐time monitoring of chloramines in drinking water, swimming pools and food processing plants. However, once the isobaric overlaps from water cluster ions are reduced at the higher temperatures, there is no conclusive evidence showing the presence of haloamines on single breath exhalations in the mid parts per trillion range from examination of the breaths of volunteers. Copyright © 2010 John Wiley & Sons, Ltd. 相似文献
85.
86.
Discovery and Structure Determination of an Unusual Sulfide Telluride through an Effective Combination of TEM and Synchrotron Microdiffraction
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Felix Fahrnbauer Dr. Tobias Rosenthal Tilo Schmutzler Priv.‐Doz. Dr. Gerald Wagner Dr. Gavin B. M. Vaughan Dr. Jonathan P. Wright Prof. Dr. Oliver Oeckler 《Angewandte Chemie (International ed. in English)》2015,54(34):10020-10023
The structure elucidation of the novel sulfide telluride Pb8Sb8S15Te5 demonstrates a new versatile procedure that exploits the synergism of electron microscopy and synchrotron diffraction methods for accurate structure analyses of side‐phases in heterogeneous microcrystalline samples. Suitable crystallites of unknown compounds can be identified by transmission electron microscopy and relocated and centered in a microfocused synchrotron beam by means of X‐ray fluorescence scans. The refined structure model is then confirmed by simulating HRTEM images of the same crystallite. Pb8Sb8S15Te5 consists of chains of heterocubane‐like units. Cation coordination polyhedra form unusually entwined chains of edge‐ and face‐sharing bicapped trigonal prisms. The structure data are precise enough for bond‐valence calculations, which confirm the disordered atom distribution. On this basis, optimization of physical properties becomes feasible. 相似文献
87.
The siting of Cu2+ in zeolites with low exchange levels has been a subject for debate due to the lack of experimental evidence that provide directly the interaction between the Cu2+ ion and the zeolite framework. High field 27Al ENDOR provided highly resolved orientation selective ENDOR spectra from which both the 27Al hyperfine and quadrupole principal components and orientations relative to the g tensor principal axis system were determined for a dehydrated Cu2+ exchanged zeolite X with Si/Al = 1. The results show that all three Cu-Al distances in the six-member ring are equivalent, in contrast to DFT predictions using cluster models. 相似文献
88.
Roth A Becher J Herrmann C Görls H Vaughan G Reiher M Klemm D Plass W 《Inorganic chemistry》2006,45(25):10066-10076
The trinuclear copper(II) complexes ([CuL1)(mu-ac)Cu(mu-ac)CuL1) (1) and ([CuL2)(mu-ac)Cu(mu-ac)CuL2) (2) of the tridentate aminosaccharide-derived Schiff-base ligands H2L1 [6-N-(salicylidene)amino-6-deoxy-1,2,3-tri-O-methyl-alpha-D-glucopyranoside] and H2L2 [6-N-(3,5-di-tert-butylsalicylidene)amino-6-deoxy-1,2,3-tri-O-methyl-alpha-D-glucopyranoside] were synthesized and structurally characterized. The trinuclear complex units can be described as two terminal copper-ligand moieties bridged by a central copper acetate moiety, with the Cu centers arranged in a triangular fashion. IR and UV/vis spectroscopic studies strongly indicate that the trinuclear structure is maintained in a methanolic solution. The temperature dependence of the magnetic susceptibility of both complexes shows a moderate antiferromagnetic coupling and can be well interpreted by applying a symmetric Cua-Cub-Cua' model with linear spin topology. The fit of the magnetic data affords coupling constants J of -34 and -24 cm(-1) for 1 and 2, respectively [H = -J(SaSb + SbSa')]. For mu-alkoxo-mu-acetato-bridged copper(II) complexes with a large dihedral angle between the adjacent coordination planes, as found in 1 and 2, such an antiferromagnetic coupling is unusual. However, density functional theory calculations of 2 using BP86, B3LYP*, and B3LYP density functionals confirmed a symmetric doublet ground state. 相似文献
89.
Let f(n) be a totally multiplicative function such that | ƒ (n)|⪯ 1 for all n, and let F(s) = ∑ ∞ n=1 ƒ(n)n —∞ be the associated Dirichlet series. A variant of Halász"s method is developed, by means of which estimates for ∑ N n=1 ƒ(n)/n are obtained in terms of the size of | F(s) | for s near 1 with ℜs >1. The result obtained has a number of consequences, particularly concerning the zeros of the partial sum U N (s) =∑ N n=1 n-s s of the series for the Riemann zeta function. 相似文献
90.
D. Vaughan Griffiths Helen J. Groombridge Stephen P. Swetnam David C. York 《Tetrahedron》2005,61(19):4595-4600
The synthesis of a range of new phosphine-containing polydentate ligands has been achieved by addition of sulfur and nitrogen nucleophiles to dimethylvinylphosphine sulfide, followed by reduction of the resulting phosphine sulfides with lithium aluminium hydride. 相似文献