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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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《Ceramics International》2022,48(17):24383-24392
We propose a novel approach for manufacturing dual-scale porosity alumina structures by UV curing-assisted 3D plotting of a specially formulated alumina feedstock using a thermo-regulated phase separable, photocurable camphene/triethylene glycol dimethacrylate (TEGDMA) vehicle. In particular, 3D plotting process was conducted at - 5 °C, and thus an alumina suspension prepared using liquid camphene/TEGDMA at room temperature could undergo phase separation, resulting in camphene crystals surrounded by walls comprised of liquid photopolymer enclosing alumina particles. To enhance the shape retention ability of extruded filaments, polystyrene (PS) polymer was used as the tackifier. The phase-separated feedrod could be extruded favorably through a nozzle and rapidly photopolymerized by UV light during the 3D plotting process. Three-dimensionally interconnected macropores were tightly constructed, which were separated by microporous alumina filaments, where micropores were created by the removal of camphene crystals via freeze-dying. The macroporosity of porous alumina ceramics was controlled by adjusting the distance between deposited filaments, while their microporosity was kept constant, leading to tightly tailored overall porosity and mechanical properties.  相似文献   
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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   
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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   
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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   
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Proper management of the liquid water and heat produced in proton exchange membrane (PEM) fuel cells remains crucial to increase both its performance and durability. In this study, a two-phase flow and multicomponent model, called two-fluid model, is developed in the commercial COMSOL Multiphysics® software to investigate the liquid water heterogeneities in large area PEM fuel cells, considering the real flow fields in the bipolar plate. A macroscopic pseudo-3D multi-layers approach has been chosen and generalized Darcy's relation is used both in the membrane-electrode assembly (MEA) and in the channel. The model considers two-phase flow and gas convection and diffusion coupled with electrochemistry and water transport through the membrane. The numerical results are compared to one-fluid model results and liquid water measurements obtained by neutron imaging for several operating conditions. Finally, according to the good agreement between the two-fluid and experimentation results, the numerical water distribution is examined in each component of the cell, exhibiting very heterogeneous water thickness over the cell surface.  相似文献   
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Polarization imaging can retrieve inaccurate objects’ 3D shapes with fine textures, whereas coarse but accurate depths can be provided by binocular stereo vision. To take full advantage of these two complementary techniques, we investigate a novel 3D reconstruction method based on the fusion of polarization imaging and binocular stereo vision for high quality 3D reconstruction. We first generate the polarization surface by correcting the azimuth angle errors on the basis of registered binocular depth, to solve the azimuthal ambiguity in the polarization imaging. Then we propose a joint 3D reconstruction model for depth fusion, including a data fitting term and a robust low-rank matrix factorization constraint. The former is to transfer textures from the polarization surface to the fused depth by assuming their relationship linear, whereas the latter is to utilize the low-frequency part of binocular depth to improve the accuracy of the fused depth considering the influences of missing-entries and outliers. To solve the optimization problem in the proposed model, we adopt an efficient solution based on the alternating direction method of multipliers. Extensive experiments have been conducted to demonstrate the efficiency of the proposed method in comparison with state-of-the-art methods and to exhibit its wide application prospects in 3D reconstruction.  相似文献   
10.
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   
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