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61.
The experimental part of this study focuses on FTIR spectroscopy of SO(2) adsorbate on the surface of ice nanoparticles at 128 K, in the 0.5-1 monolayer coverage range. In addition to the infrared spectroscopic features due to molecular SO(2), a structured band is observed at approximately 1030 cm(-1). A similar band was observed in past spectroscopic studies of SO(2) aqueous solutions, and assigned to anionic products of SO(2) ionization. Ab initio normal mode analysis of HSO(3)(-) yielded intense SO stretch bands in the vicinity of the observed "ionic" feature. The relative intensities of the molecular and the anionic bands indicate that 0.3 approximately 0.5 of the adsorbate is ionized. These results are consistent with the previously published data on isotopic exchange in SO(2)-covered ice nanoparticles (Devlin and Buch, J. Chem. Phys., 2007, 127, 091101) which pointed towards substantial SO(2) ionization at low temperatures. Density functional theory modeling of molecular and ionized adsorbate on a crystal ice slab suggests that anion solvation by molecular SO(2) adsorbate facilitates the SO(2) ionization process at the ice surface.  相似文献   
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This article refers to the mineralogical composition and phase transformations of Greek nickeliferous laterites and to their metallurgical behaviour, during preheating and reduction with carbon monoxide. Transformation of goethite to hematite and decomposition of chlorite and serpentine, were identified during preheating. Higher iron metallization was achieved for the ore in which goethite is the main iron mineral and reduction goes up to 95%, whereas it goes up to 50% for the ore in which hematite is the main iron mineral. The higher reducibility, however, seems to be due to the higher specific surface area of the goethitic type of ore.  相似文献   
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Klencsár  Z.  Kuzmann  E.  Homonnay  Z.  Vértes  A.  Simopoulos  A.  Devlin  E.  Kallias  G. 《Hyperfine Interactions》2002,144(1-4):261-266
Hyperfine Interactions - The temperature dependence of the local electronic and magnetic state of iron in the chalcogenide spinel FeCr2S4 has been studied in detail around the Curie temperature...  相似文献   
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Low-temperature, low-pressure studies of clathrate hydrates (CHs) have revealed that small ether and other proton-acceptor guests greatly enhance rates of clathrate hydrate nucleation and growth; rapid formation and transformations are enabled at temperatures as low as 110 K, and cool moist vapors containing small ether molecules convert to mixed-gas CHs on a subsecond time scale. More recently, FTIR spectroscopic studies of the tetrahydrofuran (THF)-HCN double clathrate hydrate revealed a sizable frequency shift accompanied by a four-fold intensification of the C-N stretch-mode absorption of the small cage HCN, behavior that is enhanced by cooling and which correlates precisely with similar significant changes of the ether C-O/C-C stretch modes. These temperature-dependent correlated changes in the infrared spectra have been attributed to equilibrated extensive hydrogen bonding of neighboring large- and small-cage guest molecules with water molecules of the intervening wall. An ether guest functions as a proton acceptor, particularly so when complemented by the action of a proton-donor (HCN)/electron-acceptor (SO(2)) small-cage guest. Because guest molecules of the classic clathrate hydrates do not participate in hydrogen bonds with the host water, this H-bonding of guests has been labeled "nonclassical". The present study has been enriched by comparing observed FTIR spectra with high-level molecular orbital computational results for guests and hydrogen-bonded guest-water dimers. Vibrational frequency shifts, from heterodimerization of ethers and water, correlate well with the corresponding observed classical to nonclassical shifts. The new spectroscopic data reveal that the nonclassical structures can contribute at observable levels to CH infrared spectra for a remarkable range of temperatures and choice of guest molecules. By the choice of guest molecules, it is now possible to select the abundance levels of nonclassical configurations, ranging from ~0 to 100%, for a given temperature. This ability is expected to hasten understanding of the role of guest-induced nonclassical structures in the acceleration or inhibition of the rates of CH formation and transformation.  相似文献   
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Six [Fe(8)(μ(4)-O)(4)(μ-4-R-pyrazolato)(12)X(4)] complexes containing an identical Fe(8)(μ(4)-O)(4) core have been structurally characterized and studied by M?ssbauer spectroscopy. In each case, an inner μ(4)-O bridged Fe(III) cubane core is surrounded by four trigonal bipyramidal iron centers, the two distinct sites occurring in a 1:1 ratio. The M?ssbauer spectrum of each of the clusters consists of two quadrupole doublets, which, with one exception (X = NCS, R = H), overlap to give three absorption lines. The systematic variation of X and R causes significant changes in the M?ssbauer spectra. A comparison with values for the same clusters computed using density functional theory allows us to establish an unequivocal assignment of these peaks in terms of a nested model for the overlapping doublets. The changes in M?ssbauer parameters (both experimental and computed) for the 1-electron reduced species [Fe(8)(μ(4)-O)(4)(μ-4-Cl-pyrazolato)(12)Cl(4)](-) are consistent with a redox event that is localized within the cubane core.  相似文献   
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For the first time, measurements of the cosmic microwave background radiation (CMB) alone favor cosmologies with w = -1 dark energy over models without dark energy at a 3.2-sigma level. We demonstrate this by combining the CMB lensing deflection power spectrum from the Atacama Cosmology Telescope with temperature and polarization power spectra from the Wilkinson Microwave Anisotropy Probe. The lensing data break the geometric degeneracy of different cosmological models with similar CMB temperature power spectra. Our CMB-only measurement of the dark energy density Ω(Λ) confirms other measurements from supernovae, galaxy clusters, and baryon acoustic oscillations, and demonstrates the power of CMB lensing as a new cosmological tool.  相似文献   
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