The demand for dielectric capacitors with higher energy-storage capability is increasing for power electronic devices due to the rapid development of electronic industry. Existing dielectrics for high-energy-storage capacitors and potential new capacitor technologies are reviewed toward realizing these goals. Various dielectric materials with desirable permittivity and dielectric breakdown strength potentially meeting the device requirements are discussed. However, some significant limitations for current dielectrics can be ascribed to their low permittivity, low breakdown strength, and high hysteresis loss, which will decrease their energy density and efficiency. Thus, the implementation of dielectric materials for high-energy-density applications requires the comprehensive understanding of both the materials design and processing. The optimization of high-energy-storage dielectrics will have far-reaching impacts on the sustainable energy and will be an important research topic in the near future.
We have studied the optical properties (complex dielectric function) of bulk SrTiO3 and thin films on Si and Pt using spectroscopic ellipsometry over a very broad spectral range, starting at 0.03 eV [using Fourier transform infrared (FTIR) ellipsometry] to 8.7 eV. In the bulk crystals, we analyze the interband transitions in the spectra to determine the critical-point parameters. To interpret these transitions, we performed band structure calculations based on ab initio pseudopotentials within the local-density approximation. The dielectric function was also calculated within this framework and compared with our ellipsometry data. In the FTIR ellipsometry data, we notice a strong lattice absorption peak due to oxygen-related vibrations. Two longitudinal optic (LO) phonons were also identified. In SrTiO3 films on Si, the refractive index below the band gap decreases with decreasing thickness because of the increasing influence of the amorphous interfacial layer between the SrTiO3 film and the Si substrate. There is also a decrease in amplitude and an increase in broadening of the critical points with decreasing thickness. In SrTiO3 films on Pt, there is a strong correlation between the crystallinity and texture of the films (mostly aligned with the Pt pseudosubstrate) and the magnitude of the refractive index, the Urbach tail below the bulk band edge, and the critical-point parameters. FTIR reflectance measurements of SrTiO3 on Pt (reflection–absorption spectroscopy) show absorption peaks at the LO phonon energies, a typical manifestation of the Berreman effect for thin insulating films on a metal. The Urbach tail in our ellipsomety data and the broadening of the optical phonons in SrTiO3 on Pt are most likely caused by oxygen vacancy clusters.
A series of cobalt complexes of 5,10,15-tris(pentafluorophenyl)-corrole [Co(tpfc)] (1) with various axial ligands were synthesized and examined as single-site catalysts for water oxidation. The used axial ligands include 4-cyanopyridine (py-CN), pyridine (py), 4-(dimethylamino)pyridine (py-NMe), 4-methoxypyridine (py-OMe), 1-methylimidazole (im-Me), and thiophenolate (thi). Complexes 1-py and 1-py-OMe were structurally characterized. The Co ion in both structures has an almost identical distorted octahedral coordination environment with the four N atoms of tpfc defining the equatorial plane and the two molecules of pyridine (for 1-py) or 4-methoxypyridine (for 1-py-OMe) occupying the axial positions. Electrochemical studies of these Co corroles in acetonitrile showed that they all display two oxidation events and the oxidation waves shift to the cathodic direction with electron-donating axial ligands, a trend that is consistent with increased electron densities on Co ions. All these Co corroles were found to be active for electrocatalytic water oxidation: by using catalyst-coated fluorine-doped tin oxide (FTO) working electrodes, cyclic voltammograms displayed pronounced catalytic waves for water oxidation in 0.1 M pH 7.0 phosphate buffer solutions. The onset overpotentials are in the range of 510 to 580 mV, depending on the electron-donating ability of the trans axial ligands. These results demonstrate that the catalytic activities of Co corroles for water oxidation are considerably affected by the trans axial ligands on Co centers and provide valuable insights into the design of new catalysts for water oxidation.
Isobutanol serves as an ideal gasoline additive owing to its good compatibility with current engine technology, high energy density, and high octane number. Herein, an efficient and selective Mn‐catalyzed upgrading of ethanol with methanol into isobutanol is reported. This is the first example of deoxygenative coupling of lower alcohols to isobutanol by using a homogeneous non‐noble‐metal catalyst. This transformation proceeded at very low catalyst loading with a high turnover number (9233) and up to 96 % isobutanol selectivity.
Searching
for highly efficient oxygen reduction reaction (ORR)
electrocatalysts for fuel cell technology, in which the crystal structure
plays a powerful role in regulating the electrocatalysis, is urgent
yet challenging. Herein, we have explored the active and stable Pd–Se
alloy electrocatalysts with controlled phase toward alkaline ORR.
The phase-controlled Pd–Se nanoparticles (NPs) show interesting
phase-dependent electrocatalytic performance, in which the Pd17Se15 NPs/C exhibits much better ORR performance
than its counterpart, Pd7Se4 NPs/C, and the
commercial Pd/C and Pt/C. Based on the detailed analysis, Pd in Pd17Se15 possesses more Se atom coordination and a
higher valence state, thus providing a stronger capacity for the absorption
of oxygenated species. DFT further reveals more charge transfer from
the Pd17Se15 surface to the *OOH intermediate,
which is the reason for the activity enhancement.
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