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51.
Conrad A. P. Goodwin Dr. Floriana Tuna Prof. Eric J. L. McInnes Prof. Stephen T. Liddle Dr. Jonathan McMaster Dr. Inigo J. Vitorica‐Yrezabal Dr. David P. Mills 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(45):14579-14583
We report the synthesis and characterization of the uranium(III) triamide complex [UIII(N**)3] [ 1 , N**=N(SiMe2tBu)2?]. Surprisingly, complex 1 exhibits a trigonal planar geometry in the solid state, which is unprecedented for three‐coordinate actinide complexes that have exclusively adopted trigonal pyramidal geometries to date. The characterization data for [UIII(N**)3] were compared with the prototypical trigonal pyramidal uranium(III) triamide complex [UIII(N“)3] (N”=N(SiMe3)2?), and taken together with theoretical calculations it was concluded that pyramidalization results in net stabilization for [UIII(N“)3], but this can be overcome with very sterically demanding ligands, such as N**. The planarity of 1 leads to favorable magnetic dynamics, which may be considered in the future design of UIII single‐molecule magnets. 相似文献
52.
Vijay S. Parmar Dr. Fabrizio Ortu Dr. Xiaozhou Ma Dr. Nicholas F. Chilton Dr. Rodolphe Clérac Dr. David P. Mills Prof. Dr. Richard E. P. Winpenny 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(35):7774-7778
A new family of five-coordinate lanthanide single-molecule magnets (Ln SMMs) [Dy(Mes*O)2(THF)2X] (Mes*=2,4,6-tri-tert-butylphenyl; X=Cl, 1 ; Br, 2 ; I, 3 ) is reported with energy barriers to magnetic reversal >1200 K. The five-coordinate DyIII ions have distorted square pyramidal geometries, with halide anions on the apex, and two Mes*O ligands mutually trans- to each other, and the two THF molecules forming the second trans- pair. These geometrical features lead to a large magnetic anisotropy in these complexes along the trans-Mes*O direction. QTM and Raman relaxation times are enhanced by varying the apex halide from Cl to Br to I, or by dilution in a diamagnetic yttrium analogue. 相似文献
53.
Kevin Henbest Peter Douglas Michael S. Garley Andrew Mills 《Journal of photochemistry and photobiology. A, Chemistry》1994,80(1-3):299-305
The rate constant for the reaction between the sulphate radical (SO4√−) and the ruthenium (II) tris-bipyridyl dication (Ru(bipy)32+) is (3.3±0.2)×109 mol−1 dm3 s−1 in 1 mol dm−3 H2SO4 and (4.9±0.5)×109 mol−1 dm3 s−1 in 0.1 mol dm−3, pH 4.7 acetate buffer. The SO4√−radical produced by the electron transfer quenching of Ru(bipy)32+* by S2O82− reacts rapidly with both acetate buffer and chloride ions. These side reactions result in a reduction in the overall quantum yield of Ru(bipy)33+ production and reduced reaction selectivity when Ru(bipy)32+* is quenched by persulphate. 相似文献
54.
The compressive stress relaxation modulus of a container glass composition was investigated over a wide range of strain, time, modulus, and temperature. It is shown that the glass behaves in a linear viscoelastic manner up to a 2% strain level, and that the relaxation modulus is a smooth function of time, with no pseudo-rubbery plateau apparent down to a modulus of 108 dyn/cm2. The data cover roughly five decades of modulus, five decades of time, and a temperature range of 150° C above the glass transition, Tg = 536°C. Within experimental error, the effect of temperature on the stress relaxation behavior is to simply shift the modulus-time curves along the time axis with no change in shape. Temperature dependent shift factor data are expressed in terms of the WLF relation, and are shown to be in good agreement with data found in the literature for other silicate compositions. Viscosity data derived from the generated stress relaxation data agree well with data obtained by more direct methods. 相似文献
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QSAR modeling of flotation collectors using principal components extracted from topological indices 总被引:1,自引:0,他引:1
Natarajan R Nirdosh I Basak SC Mills DR 《Journal of chemical information and computer sciences》2002,42(6):1425-1430
Several topological indices were calculated for substituted-cupferrons that were tested as collectors for the froth flotation of uranium. The principal component analysis (PCA) was used for data reduction. Seven principal components (PC) were found to account for 98.6% of the variance among the computed indices. The principal components thus extracted were used in stepwise regression analyses to construct regression models for the prediction of separation efficiencies (Es) of the collectors. A two-parameter model with a correlation coefficient of 0.889 and a three-parameter model with a correlation coefficient of 0.913 were formed. PCs were found to be better than partition coefficient to form regression equations, and inclusion of an electronic parameter such as Hammett sigma or quantum mechanically derived electronic charges on the chelating atoms did not improve the correlation coefficient significantly. The method was extended to model the separation efficiencies of mercaptobenzothiazoles (MBT) and aminothiophenols (ATP) used in the flotation of lead and zinc ores, respectively. Five principal components were found to explain 99% of the data variability in each series. A three-parameter equation with correlation coefficient of 0.985 and a two-parameter equation with correlation coefficient of 0.926 were obtained for MBT and ATP, respectively. The amenability of separation efficiencies of chelating collectors to QSAR modeling using PCs based on topological indices might lead to the selection of collectors for synthesis and testing from a virtual database. 相似文献
58.
Psychometric functions for gap detection in noise measured from young and aged subjects. 总被引:3,自引:0,他引:3
N J He A R Horwitz J R Dubno J H Mills 《The Journal of the Acoustical Society of America》1999,106(2):966-978
Psychometric functions for gap detection of temporal gaps in wideband noise were measured in a "yes/no" paradigm from normal-hearing young and aged subjects with closely matched audiograms. The effects of noise-burst duration, gap location, and uncertainty of gap location were tested. A typical psychometric function obtained in this study featured a steep slope, which was independent of most experimental conditions as well as age. However, gap thresholds were generally improved with increasing duration of the noise burst for both young and aged subjects. Gap location and uncertainty had no significant effects on the thresholds for the young subjects. For the aged subjects, whenever the gap was sufficiently away from the onset or offset of the noise burst, detectability was robust despite uncertainty about the gap location. Significant differences between young and aged subjects could be observed only when the gap was very close to the signal onset and offset. 相似文献
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60.
Talat S. Rahman D.L. Mills J.E. Black 《Journal of Electron Spectroscopy and Related Phenomena》1983,29(1):199-212
Electron energy loss spectroscopy has proved a powerful probe of vibrational modes of a wide variety of adsorbed species. Here the primary focus has been on modes with frequency well above the maximum phonon frequency of the substrate. Examples are internal vibration modes of adsorbed molecules, possibly shifted significantly in frequency from their gas phase analogues, and high frequency vibrations of an adsorbed molecule or atom against the substrate. Recent experiments explore features in the energy loss spectrum with frequency below the maximum phonon frequency of the substrate, for ordered overlayers of atoms adsorbed on low index metal surfaces. We shall summarize our theoretical studies of such spectra for several adsorbate/substrate combinations, with emphasis oh the physical origin of the features which appear in the calculations. We obtain a good account of the existing data, within the framework of a rather simple lattice dynamical model, and the calculations show that the features which appear are quite sensitive to the symmetry of the adsorption sits, and other details of the surface geometry. We shall illustrate this with several specific examples. 相似文献