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1.
We report the precise postsynthetic control of the composition of β‐Fe1+xSe by electrochemistry with simultaneous tracking of the associated structural changes via in situ synchrotron X‐ray diffraction. We access the full phase width of 0.01<x<0.04 and identify the superconducting state below 8 K, which in contrast to earlier reports is independent of the composition. However, in a second set of in situ X‐ray diffraction experiments, we demonstrate that β‐Fe1+xSe forms a new phase in the presence of oxygen above a 100 °C which has the same anti‐PbO type structure but is not superconducting down to 1.8 K. The latter process can be reversed electrochemically to reinstate the superconducting state. These observations exploit the exquisite control afforded by electrochemistry in contrast with classical approaches of chemical synthesis.  相似文献   
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Rotational spectra of ortho-nitrotoluene (2-NT) and para-nitrotoluene (4-NT) have been recorded at low and room temperatures using a supersonic jet Fourier Transform microwave (MW) spectrometer and a millimeter-wave frequency multiplier chain, respectively. Supported by quantum chemistry calculations, the spectral analysis of pure rotation lines in the vibrational ground state has allowed to characterise the rotational energy, the hyperfine structure due to the 14N nucleus and the internal rotation splittings arising from the methyl group. For 2-NT, an anisotropic internal rotation of coupled −CH3 and −NO2 torsional motions was identified by quantum chemistry calculations and discussed from the results of the MW analysis. The study of the internal rotation splittings in the spectra of three NT isomers allowed to characterise the internal rotation potentials of the methyl group and to compare them with other mono-substituted toluene derivatives in order to study the isomeric influence on the internal rotation barrier.  相似文献   
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This paper intensively investigated the ignition of turbulent coal flames in a novel fully-mixed tubular swirl burner. The Nikon D300s digital camera was used to capture the statistical ignition behavior of dispersed coal particle streams in different ambiences. Meanwhile, the combustion dynamics of individual coal particles were also recorded by means of high-speed photography. Two low-rank coal samples, Hulunbel lignite and Zhundong coal, were tested in this study. The ignition delay times of coal particles in the swirl burner were compared with those in a flat-flame burner. In contrast to previous work on a laminar flat-flame burner, the current experimental results show that the turbulent ambience significantly enhances the ignition of all coal samples, which is exceptionally pronounced under high temperature and low oxygen conditions. In addition, the sensitivity analysis suggests that both the enhanced heat and mass transfer contribute to the early ignition in turbulence. The effect of elevated mass transfer coefficient turns prominent in low oxygen fraction ambience, wherein the volatile barrier effect is suppressed by the enhanced mixing process. The combined effect of turbulence favors the shifting of ignition modes to the heterogeneous-dominant region. Last but not least, the ceased volatile flame that visualized in turbulent low oxygen ambience further confirms the important role of heterogeneous ignition.  相似文献   
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The rotational spectrum of isoamyl acetate, H3C–COO–(CH2)2–CH(CH3)2, has been recorded and assigned using a molecular beam Fourier transform microwave (MB-FTMW) spectrometer in the frequency range of 3–26.5?GHz. One conformer has been observed. By comparing the spectroscopic data with the quantum chemical data, it was found that the conformer observed does not have Cs symmetry. The rotational and centrifugal distortion constants were determined. The barrier to internal rotation of the acetate methyl group was found to be 93.98?cm?1. Due to the high number of the conformers, a systematic nomenclature will be presented.  相似文献   
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Formation of crack arrays plays an increasing role in several fields of applied physics. The energy-release rate of the cracks controls the development of the array. Therefore, following the concept of configurational forces, a simplified analytical expression is provided for the energy-release rate, which is based both on numerical studies and on a specially adapted beam model. Comparisons of this easy-to-use estimate of the energy-release rate with established results from the literature as well as detailed numerical results are presented. The provided estimate of the energy-release rate can easily be extended to non-equidistant cracks and an anisotropic material.  相似文献   
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