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1.
Borazine rings act as a pivotal part in siliconboroncarbonitride ceramics (SiBCN) for high-temperature stability and great resistance to crystallization. A detailed investigation of the ring formation mechanism will guide the design and synthesis of SiBCN to meet application requirements under extreme conditions. Boron trichloride (BCl3) and hexamethyldisilazane (HN(SiMe3)2) are common raw materials for the synthesis of precursors for SiBCN. In this paper, quantum chemical calculation was used to study the cyclization reaction mechanism between BCl3 and HN(SiMe3)2 to form trichloroborazine (TCBZ) at the MP2/6-31G (d,p) level of theory. We discussed the structure properties, reaction pathways, energy barriers, reaction rates, and other aspects in detail. The results show that BCl3 and HN(SiMe3)2 alternately participate in the reaction process, accompanied by the release of trimethylchlorosilane (TMCS), and that the entire reaction shows an absolute advantage in terms of energy. In the Step by step reaction, lower reaction barriers are formed due to the introduction of BCl3 with more heat released compared to that for the introduction of HN(SiMe3)2. The final single-molecule cyclization and TMCS elimination steps are found to be faster compared to all previous bimolecular reactions. 相似文献
2.
《Ceramics International》2022,48(8):11265-11272
Three dimensional silica mesh structures are prepared through a new and simple method for enhancing the quantum dot sensitized solar cells performance and stability.Silica patterns are made on the top of the TiO2 photoanodes and a marked improvement in light scattering properties of meshed structures is confirmed by diffuse reflectance spectroscopy measurements. This improvement enhances the current density and consequently the cells ‘efficiency. Parameters of electron transport in cells are explored by electrochemical impedance spectroscopy (EIS). According to the EIS results, silica mesh declines the recombination rate in cells in a clear way. Here more than 50% efficiency improvement is obtained in meshed structures in comparison to cells with normal TiO2 photoanode structures. The insulated silica mesh, reduces the electrolyte's deleterious effect on the semiconductor layers and the cells’ stability is improved. 相似文献
3.
《International Journal of Hydrogen Energy》2022,47(94):39864-39874
The reaction of H2 and O2 to water are studied over a Ag–Pd/TiO2 anatase catalyst, under dark and photo-irradiation conditions in the gas and liquid phases. The catalyst consisted of metal particles of mean size of ca.1 nm dispersed over 10–15 nm TiO2 particles. Kinetic parameters including order of reaction (n), rate constant (k), and activation energy (Ea), were evaluated. Ea for the thermal reaction was found to be 49-47 kJ mol?1. The oxidation reaction rate constant was found to be ca. 3 times higher in the presence of photons when compared to dark reaction at room temperature. The overall quantum yield of the reaction in the slurry phase was found to be 0.09. Considering the number of metal particles on TiO2, the photon yield per metal particle was found to be 0.16. A possible explanation of the changes in kinetics with respect to experimental conditions is given. 相似文献
4.
Robust excitation of a large spin ensemble is a long-standing problem in the field of quantum information science and engineering and presents a grand challenge in quantum control. A formal theoretical treatment of this task is to formulate it as an ensemble control problem defined on an infinite-dimensional space. In this paper, we present a distinct perspective to understand and control quantum ensemble systems. Instead of directly analyzing spin ensemble systems defined on a Hilbert space, we transform them to a space where the systems have reduced dimensions with distinctive network structures through the introduction of moment representations. In particular, we illustrate the idea of moment quantization for a spin ensemble and illuminate how this technique leads to a dynamically equivalent control system of moments. This equivalence enables the control of spin ensembles through the control of their moment systems, which in turn creates a new control analysis and design paradigm for quantum ensemble systems based on the use of truncated moment systems. 相似文献
5.
《International Journal of Hydrogen Energy》2022,47(99):41783-41794
To satisfy arising energy needs and to handle the forthcoming worldwide climate transformation, the major research attention has been drawn to environmentally friendly, renewable and abundant energy resources. Hydrogen plays an ideal and significant role is such resources, due to its non-carbon based energy and production through clean energy. In this work, we have explored catalytic activity of a newly predicted haeckelite boron nitride quantum dot (haeck-BNQD), constructed from the infinite BN sheet, for its utilization in hydrogen production. Density functional theory calculations are employed to investigate geometry optimization, electronic and adsorption mechanism of haeck-BNQD using Gaussian16 package, employing the hybrid B3LYP and wB97XD functionals, along with 6–31G(d,p) basis set. A number of physical quantities such as HOMO/LUMO energies, density of states, hydrogen atom adsorption energies, Mulliken populations, Gibbs free energy, work functions, overpotentials, etc., have been computed and analysed in the context of the catalytic performance of haeck-BNQD for the hydrogen-evolution reaction (HER). Based on our calculations, we predict that the best catalytic performance will be obtained for H adsorption on top of the squares or the octagons of haeck-BNQD. We hope that our prediction of most active catalytic sites on haeck-BNQD for HER will be put to test in future experiments. 相似文献
6.
7.
Xin Xie Yunhua Yang Yong-Hao Xiao Xiaomo Huang Qingshan Shi Wei-De Zhang 《International Journal of Hydrogen Energy》2018,43(14):6954-6962
Owing to its up-conversion photoluminescence, photo-induced electron transfer property, and excellent conductivity, carbon quantum dots (CQDs) have been established as effective sensitizers in combination with Fe2O3 nanowires for enhancing the catalytic activity of photoelectrochemical water oxidation. In comparison to pristine Fe2O3 nanowires, Fe2O3 nanowires decorated with CQDs demonstrate 27 orders of magnitude increase in photocurrent density at 0.23 V vs. Ag/AgCl. The mechanism of enhanced photoelectrochemical activity of CQDs/Fe2O3 composite was also investigated. Thereby, it is confirmed that the enhanced optical absorption, accelerated interfacial charge carrier transfer and effective separation of photogenerated electron-hole pairs induced by CQDs decoration account for the enhancement of CQDs/Fe2O3 nanowire arrays in photoelectrochemical application. 相似文献
8.
《Ceramics International》2020,46(1):17-22
Au/SnO2 quantum dots (AuSQDs) were synthesized, and the effects of annealing on their structural and optical properties were examined. Significant changes were observed in the bandgap and surface plasmon resonance (SPR) of the AuSQDs after thermal treatment at different temperatures (400, 500, and 600 °C). The properties of the as-prepared and annealed samples were characterized via X-ray diffraction analysis, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy, and diffuse reflectance spectroscopy. Annealing reduced the bandgap from 3.03 to 2.33 eV and increased the crystallinity while maintaining an average crystallite size below 10 nm. XPS valence band (VB) profiles provided information regarding the VB edge potentials, which helped to determine the conduction band edge potentials. An enhancement in the SPR of the Au nanoparticles was observed for AuSQD-500, which had the smallest bandgap among the samples investigated. 相似文献
9.
Jialiang Pan Ziying Guo Zhenpeng Zhu Zishan Sun Tingting Zhang Jilin Zhang Xinguo Zhang 《Ceramics International》2018,44(17):20732-20738
High-efficient Ce3+/Tb3+ co-doped Ba3Y2B6O15 phosphors with multi color-emitting were firstly prepared, and their structural and luminescent properties were studied by XRD Rietveld refinement, emission/excitation spectra, fluorescence lifetimes as well as temperature-variable emission spectra. Upon 365?nm excitation, the characteristic blue Ce3+ band along with green Tb3+ peaks were simultaneously found in the emission spectra. Moreover, by increasing concentration of Tb3+, a blue-to-green tunable emitting color could be realized by effective Ce3+→Tb3+ energy transfer. Furthermore, all Ba3Y2B6O15: Ce3+, Tb3+ phosphors exhibit high internal quantum efficiency of ~?90%, while the temperature-variable emission spectra reveal that the phosphors possess impressive color stability as well as good thermal stability (T50 =?~?120?°C). The results indicate that these efficient color-tuning Ba3Y2B6O15: Ce3+, Tb3+ might be candidate as converted phosphor for UV-excited light-emitting diodes. 相似文献
10.
Over the last decade, narrow-band emitters have been recognized as key enablers for light emitting diodes (LEDs) backlights in liquid-crystal displays (LCDs) by competing with other display technologies. Today, efforts have been devoted to the exploration of narrow-band green/red luminescent materials with high quantum efficiency and excellent stability to optimize the performance of LED backlights. This review first presents an overview of the significant progress made in the development of narrow-band emitters used in LED backlights for LCDs with the emphasis on the versatile materials databases from doped phosphors to luminescent II–VI, III-V semiconductor quantum dots, and the recent halide perovskites nanocrystals and bulk metal halides. Subsequently, the correlation of structure-luminescence properties, and the device performance optimization of these emitters have been analyzed. The focus is placed on summarizing and comparing the remarkable examples of outdated and new narrow-band luminescent materials as potential candidates in LED backlights. Finally, the outlooks and challenges in discovering new narrow-band emitters have been proposed. 相似文献