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1.
Due to the demand of miniaturization and integration for ceramic capacitors in electronic components market, TiO2-based ceramics with colossal permittivity has become a research hotspot in recent years. In this work, we report that Ag+/Nb5+ co-doped (Ag1/4Nb3/4)xTi1−xO2 (ANTOx) ceramics with colossal permittivity over a wide frequency and temperature range were successfully prepared by a traditional solid–state method. Notably, compositions of ANTO0.005 and ANTO0.01 respectively exhibit both low dielectric loss (0.040 and 0.050 at 1 kHz), high dielectric permittivity (9.2 × 103 and 1.6 × 104 at 1 kHz), and good thermal stability, which satisfy the requirements for the temperature range of application of X9R and X8R ceramic capacitors, respectively. The origin of the dielectric behavior was attributed to five dielectric relaxation phenomena, i.e., localized carriers' hopping, electron–pinned defect–dipoles, interfacial polarization, and oxygen vacancies ionization and diffusion, as suggested by dielectric temperature spectra and valence state analysis via XPS; wherein, electron-pinned defect–dipoles and internal barrier layer capacitance are believed to be the main causes for the giant dielectric permittivity in ANTOx ceramics.  相似文献   
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3.
Transition metals sulfide-based nanomaterials have recently received significant attention as a promising cathode electrode for the oxygen evolution reaction (OER) due to their easily tunable electronic, chemical, and physical properties. However, the poor electrical conductivity of metal-sulfide materials impedes their practical application in energy devices. Herein, firstly nano-sized crystals of cobalt-based zeolitic-imidazolate framework (Co-ZIF) arrays were fabricated on nickel-form (NF) as the sacrificial template by a facile solution method to enhance the electrical conductivity of the electrocatalyst. Then, the Co3S4/NiS@NF heterostructured arrays were synthesized by a simple hydrothermal route. The Co-ZIFs derived Co3S4 nanosheets are grown successfully on NiS nanorods during the hydrothermal sulfurization process. The bimetallic sulfide-based Co3S4/NiS@NF-12 electrocatalyst demonstrated a very low overpotential of 119 mV at 10 mA cm?2 for OER, which is much lower than that of mono-metal sulfide NiS@NF (201 mV) and ruthenium-oxide (RuO2) on NF (440 mV) electrocatalysts. Furthermore, the Co3S4/NiS@NF-12 electrocatalyst showed high stability during cyclic voltammetry and chronoamperometry measurements. This research work offers an effective strategy for fabricating high-performance non-precious OER electrocatalysts.  相似文献   
4.
The development of efficient and stable electrocatalysts is of great significance for improving water splitting. Among them, transition metal oxyhydroxides show excellent performance in oxygen evolution reactions (OER), but there are certain difficulties in direct preparation. Recently, Metal–organic frameworks (MOFs) as precatalysts or precursors have shown promising catalytic performance in OER and can be decomposed under alkaline conditions. Therefore, using a mild and controllable way to convert MOFs into oxyhydroxides and retaining the original structural advantages is crucial for improving the catalytic activity. Herein, a rapid electrochemical strategy is used to activate well-mixed MOFs to prepare Co/Ni oxyhydroxide nanosheets for efficient OER catalysts, and the structural transformation in this process was investigated in detail by using scanning electron microscope, X-ray diffraction, Raman, X-ray photoelectron spectroscopy and electrochemical methods. It is discovered that electrochemical activation can promote ligand substitution of well-mixed MOFs to form porous oxyhydroxide nanosheets and tune the electronic structure of the metal (Co and Ni), which can lead to more active site exposure and accelerate charge transfer. In addition, the change of structure also improves hydrophilicity, as well as benefiting from the strong synergistic effect between multiple species, the optimal a-MCoNi–MOF/NF has excellent OER performance and long-term stability. More obviously, the porous CoNiOOH nanosheets are formed in situ during electrochemical activation process through structural transformation and acts as the active centers. This work provides new insights for mild synthesis of MOFs derivatives and also provides ideas for the preparation of highly efficient catalysts.  相似文献   
5.
This work investigates selective Ni locations over Ni/CeZrOx–Al2O3 catalysts at different Ni loading contents and their influences on reaction pathways in ethanol steam reforming (ESR). Depending on the Ni loading contents, the added Ni selectively interacts with CeZrOx–Al2O3, resulting in the stepwise locations of Ni over CeZrOx–Al2O3. This behavior induces a remarkable difference in hydrogen production and coke formation in ESR. The selective interaction between Ni and CeZrOx for 10-wt.% Ni generates more oxygen vacancies in the CeZrOx lattice. The Ni sites near the oxygen vacancies enhance reforming via steam activation, resulting in the highest hydrogen production rate of 1863.0 μmol/gcat·min. In contrast, for 15 and 20-wt.% Ni, excessive Ni is additionally deposited on Al2O3 after the saturation of Ni–CeZrOx interactions. These Ni sites on Al2O3 accelerate coking from the ethylene produced on the acidic sites, resulting in a high coke amount of 19.1 mgc/gcat·h (20Ni/CZ-Al).  相似文献   
6.
Hydrogen technology is widely considered a novel clean energy source, and electrolysis is an effective method for hydrogen evolution. Therefore, efficient hydrogen evolution reaction (HER) catalysts are urgently needed to replace precious metal catalysts and meet ecological and environmental protection standards. Herein, Ni–Mn–P electrocatalysts are synthesized using facile electrodeposition technology. The influence of the Mn addition on the catalytic behavior is studied by the comprehensive analysis of catalytic performance and morphology of the catalysts. Among them, the Ni–Mn–P0.01 catalyst exhibits small coral-like structures, greatly improving the adsorption and desorption of hydrogen ions and reducing the overpotential hydrogen evolution. Consequently, overpotential at 10 mA cm?2 electric current density is 113 mV, and the value of the Tafel slope achieves 74 mV/dec. Furthermore, the Ni–Mn–P catalyst shows long-time (20 h) stability at current densities of 10 and 60 mA/cm2. The results confirm that the synergistic effect of Ni, Mn, and P accelerates the electrochemical reaction. Meanwhile, the addition of manganese element can change the micromorphology of the catalyst, thereby exposing more active sites to participate in the reaction, enhancing water ionization, improving the catalytic performance. This study opens a new way toward improving the activity of the catalyst by adjusting Mn concentration during the electrodeposition process.  相似文献   
7.
Carbon dioxide (CO2) and methane (CH4) are the primary greenhouse gases (GHGs) that drive global climate change. CO2 reforming of CH4 or dry reforming of CH4 (DRM) is used for the simultaneous conversion of CO2 and CH4 into syngas and higher hydrocarbons. In this study, DRM was investigated using Ag–Ni/Al2O3 packing and Sn–Ni/Al2O3 packing in a parallel plate dielectric barrier discharge (DBD) reactor. The performance of the DBD reactor was significantly enhanced when applying Ag–Ni/Al2O3 and Sn–Ni/Al2O3 due to the relatively high electrical conductivity of Ag and Sn as well as their anti-coke performances. Using Ag–Ni/Al2O3 consisting of 1.5 wt% Ag and 5 wt% Ni/Al2O3 as the catalyst in the DBD reactor, 19% CH4 conversion, 21% CO2 conversion, 60% H2 selectivity, 81% CO selectivity, energy efficiency of 7.9% and 0.74% (by mole) coke formation were achieved. In addition, using Sn–Ni/Al2O3, consisting of 0.5 wt% Sn and 5 wt% Ni/Al2O3, 15% CH4 conversion, 19% CO2 conversion, 64% H2 selectivity, 70% CO selectivity, energy efficiency of 6.0%, and 2.1% (by mole) coke formation were achieved. Sn enhanced the reactant conversions and energy efficiency, and resulted in a reduction in coke formation; these results are comparable to that achieved when using the noble metal Ag. The decrease in the formation of coke could be correlated to the increase in the CO selectivity of the catalyst. Good dispersion of the secondary metals on Ni was found to be an important factor for the observed increases in the catalyst surface area and catalytic activities. Furthermore, the stability of the catalytic reactions was investigated for 1800 min over the 0.5 wt% Ag-5 wt% Ni/Al2O3 and 0.5 wt% Sn-5 wt% Ni/Al2O3 catalysts. The results showed an increase in the reactant conversions with an increase in the reaction time.  相似文献   
8.
Today, utility meters for water are tested for measurement behavior at stable operating conditions at specified flow rates as part of the approval process. The measurement error that occurs during start and stop or when changing between flow rates may not be taken into account. In addition, there are new technologies whose measuring behavior under real-world conditions is only known to a limited extend. To take these facts into account, a new method has been developed and tested to determine the measurement behavior of water meters under dynamic load profiles as they occur in the real application. For this purpose, a test rig for flow rate measurement was extended by a cavitation nozzle apparatus and the generation of dynamic load profiles was validated. For the cavitation nozzles used, possible factors influencing the flow rate, such as temperature and purity of the water as well as the upstream pressure were investigated. Using different types of domestic water meters, the applicability of the dynamic test procedure was demonstrated and the measurement behavior of the meters was characterised.  相似文献   
9.
Energy depletion and environmental pollution are still serious challenges for human beings. The application of hydrogen energy should be a promising strategy to address this issue. However, the hydrogen production should be one shortcoming for hydrogen energy. The hydrogen evolution reaction (HER) based on electrocatalysis is an effective way to enhance the hydrogen generation with small energy consumption under ambient conditions. Many works have been devoted to develop high performance catalysts to satisfy the HER processes. Nevertheless, the mechanism about facet-dependence and composition-dependence influence is still need to deeply study. Hereon, based on density functional theory calculations, the [100], [110], and [111] facets of NixPy (Ni3P, Ni2P, NiP, NiP2, NiP3) systems were created and their HER catalytic activity were used to reveal the underline mechanism. By analyzing the variation of Gibbs free energy, it was found that the structural composition has a greater effect on HER than the facet. Significantly, the Ni2P(111) surface with Ni/P-termination has the best HER performance for all samples in present work. Through exploring the electron transfer of H with surrounding atoms during the HER process, the H adsorption mechanism as well as its reaction mechanism has been revealed. The deep insights in this work provide an important fundamental that the contents of non-metal for compounds catalysts can heavily influence the performance of HER, which should give more guidance for designing new catalysts.  相似文献   
10.
In this investigation, low-cement castables were prepared using 70% alumina grog aggregates obtained from crushed alumina brick waste. The aggregates were thermally treated at 1550 °C for 3 h. Four types of low-cement castables were prepared with various types of aggregates (alumina grog with or without thermal treatment) and fillers (with or without zircon addition), and they were evaluated in terms of their physical, thermal, and chemical properties. Microstructural analysis via scanning electron microscopy (SEM) was performed on the castables before and after slag attack. Compared to the other fabricated castables, the thermally treated alumina grog castables with zircon showed better physical properties, such as a higher bulk density, cold crushing strength, and modulus of rupture and a lower apparent porosity and water absorption. In addition, they had a higher positive linear thermal expansion, refractoriness under load, permanent linear change, and hot modulus of rupture. The results of the SEM with energy dispersive X-ray analysis of the prepared castables confirmed that the mullite and anorthite phases were predominant when zircon was not added and the zircon–mullite phase additionally appeared upon the incorporation of zircon. A quantitative elemental analysis via X-ray fluorescence spectroscopy was employed to determine the composition of the castables. X-ray diffraction analysis showed that the alumina grog castables had a high mullite and low anorthite content, and the thermally treated alumina grog had a high anorthite, low mullite, and high zircon content. The improvement in the mechanical and thermo-mechanical properties of the castables with thermally treated alumina grog and added zircon can be attributed to the formation of the zircon–mullite phase with a low mullite phase content.  相似文献   
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