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1.
Pengfei Liang Jie Zhu Di Wu Hui Peng Xiaolian Chao Zupei Yang 《Journal of the American Ceramic Society》2021,104(6):2702-2710
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
2.
《International Journal of Hydrogen Energy》2022,47(100):41956-41973
Due to stringent environmental regulations and the limited resources of fossil-based fuels, there is an urgent demand for clean and eco-friendly energy conversion devices. These criteria appear to be met by hydrogen proton exchange membrane fuel cells (PEMFCs). PEMFCs have attracted tremendous attention on account of their excellent performance with tunable operability and good portability. Nonetheless, their practical applications are hugely influenced by the scarcity and high cost of platinum (Pt) used as electrocatalysts at both cathode and anode. Pt is also susceptible to easy catalyst poisoning. Herein, this paper reviews the progress of the research regarding the development of electrocatalysts practically used in hydrogen PEMFCs, where the corner-stone reactions are cathodic oxygen reduction reaction (ORR) and anodic hydrogen oxidation reaction (HOR). To reduce the costs of PEMFCs, lessening or eliminating the use of Pt is of prime importance. For current and forthcoming laboratory/large-scale PEMFCs, there is much interest in developing substitute catalysts based on cheaper materials. As such are non-platinum (non-Pt), non-platinum group metals (non-PGMs), metal oxides, and non-metal electrocatalysts. Hence, high-performance, state-of-the-art, and novel structured electrocatalysts as replacements for Pt are needed. 相似文献
3.
《International Journal of Hydrogen Energy》2022,47(63):27023-27031
Hexagonal boron nitride (h-BN) as a layered inorganic nonmetallic material has been widely used. Hydrogen peroxide (H2O2) modification can trigger exfoliation and afford abundant B–OH active sites at edge of h-BN, which can enhance methane activation ability. Introducing tungsten oxide (WO3) to h-BN produces a similar effect, because doping WO3 into h-BN resulted in electron transfer to N, inducing fracture of B–N bond, resulting in N vacancy (triboron center), exposing more B sites and promoting the generation of B–OH. Significantly, the introduction of WO3 on the modified h-BN dramatically increased the concentration of B–OH compared with the unmodified h-BN, because H2O2 modification weakened B–N bond. By means of XRD, TEM, XPS,EPR, FT-IR, it is proved that the high concentration of B–OH active sites contributed to activating C–H bond, thus methane conversion and CO and H2 selectivity were significantly improved. 相似文献
4.
《International Journal of Hydrogen Energy》2022,47(94):39961-39972
Micro-cracks commonly occur on the catalyst layers (CLs) during the manufacturing of catalyst coated membranes (CCMs). However, the crack shape parameters effect on CLs in-plane (IP) electronic conductivity λs is not clear. In this work, the relationship between crack parameters and the λs is obtained based on the two-dimensional (2D) multiple-relaxation time (MRT) lattice Boltzmann method (LBM). The LBM numerical model is validated by the normalized λs experiment applied on three different home-made cracked CLs, and the parameter study focus on crack width, length, quantity and phase angle are carried out. The results show that the decrease of λs has different sensitivity |k| to the parameters above. The crack width has little effect on λs decrease, and the |kw| is 0.038. However, crack arm length and quantity show more significant impact, which |kl| and |kN| are 0.753 and 0.725, respectively. The CLs with different crack propagation directions show significant anisotropy on λs, and a 53.53% decrease in λs is observed between 0° and 90° crack phase angle change. To manufacture a high electronic conductivity CL, crack initiation and migration mitigation are highly encouraged. 相似文献
5.
《International Journal of Hydrogen Energy》2022,47(1):276-291
To the best of our knowledge, this is the first time to report the preparation of a dotted nanowire arrayed by 5 nm sized palladium and nickel composite nanoparticles (denoted as PdxNiy NPs) via a hydrothermal method using NU and PdO·H2O as the starting materials. The samples prepared at the mass ratio of NU to PdO·H2O 1:1, 1:2 and 2:1 were, respectively, nominated as catalyst c1, c2 and c3. The chemical compositions of all synthesized catalysts were mainly studied by using X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), revealing that metallic Ni was one main component of all prepared catalysts. Surprisingly, the main diffraction peaks appearing in the XRD patterns of all prepared catalysts were assigned to the metallic Ni rather than the metallic Pd. Very interestingly, as indicated by the TEM images, a large number of dotted nanowires arrayed by numerous equidistant 5 nm sized nanoparticles were distinctly exhibited in catalyst c1. More importantly, when being used as electrocatalysts for EOR, all prepared catalysts exhibited an evident electrocatalytic activity towards EOR. In the cyclic voltammetry (CV) test, the peak current density of the forward peak of EOR on catalyst c1 measured at 50 mV s?1 was as high as 56.1 mA cm?2, being almost 9 times higher than that of EOR on catalyst c3 (6.3 mA cm?2). Particularly, the polarized current density of EOR on catalyst c1 at 3600 s, as indicated by the chronoamperometry (CA) experiment, was still maintained to be around 1.47 mA cm?2, a value higher than the latest reported data of 1.3 mA cm?2 (measured on the pure Pd/C electrode). Presenting a novel method to prepare dotted nanowires arranged by 5 nm sized nanoparticles and showing the significant eletrocatalytic activities of the newly prepared dotted nanowires towards EOR were the major contributions of this preliminary work. 相似文献
6.
Hui Liu Yaohui Fu Jinhai Yuan Lei Yu Zhefei Wang Quan Liu Bo Wei Xuhong Wang 《Ceramics International》2021,47(12):16570-16578
To provide a basis for the high-temperature oxidation of ultra-high temperature ceramics (UHTCs), the oxidation behavior of Zr3[Al(Si)]4C6 and a novel Zr3[Al(Si)]4C6-ZrB2-SiC composite at 1500 °C were investigated for the first time. From the calculation results, the oxidation kinetics of the two specimens follow the oxidation dynamic parabolic law. Zr3[Al(Si)]4C6 exhibited a thinner oxide scale and lower oxidation rate than those of the composite under the same conditions. The oxide scale of Zr3[Al(Si)]4C6 exhibited a two-layer structure, while that of the composite exhibited a three-layer structure. Owing to the volatilization of B2O3 and the active oxidation of SiC, a porous oxide layer formed in the oxide scale of the composite, resulting in the degradation of its oxidation performance. Furthermore, the cracks and defects in the oxide scale of the composite indicate that the reliability of the oxide scale was poor. The results support the service temperature of the obtained ceramics. 相似文献
7.
This study deals with the anodisation of titanium grade 2 in 0.5-M sulphuric acid using a pulsed signal in a unipolar regime. The electrical parameters investigated are voltage, frequency and duty cycle. The use of duty cycles with a high percentage of anodic polarisation (90%), combined with high frequencies (1000 Hz) and the higher voltage tested (220 V), favoured the establishment of a plasma regime involving strong dielectric discharges, allowing the growth of thicker oxides but with rough architecture. The corrosion resistance of the formed film has been characterised by potentiodynamic tests in 0.5-M NaBr for localised corrosion resistance and by immersion tests in 10% v/v sulphuric acid solution for a uniform corrosion assessment. Current–time curves, visual observations and electron microscope analysis (scanning electron microscopy, energy-dispersive X-ray spectroscopy) were the tools selected to provide a correlation between technological parameters and oxide growth mechanism. For localised and uniform corrosion, anodisation at 220 V with a high level of anodic polarisation (90%) and frequency (1000 Hz) was verified to be particularly advantageous. 相似文献
8.
《Ceramics International》2022,48(20):29892-29899
It is very challenging for 3D printing based on the selective laser melting (SLM) technology to obtain cermet bulk materials with high density and homogeneous microstructures. In this work, the SLM process of the cermet powders was studied by both simulations and experiments using the WC-Co cemented carbides as an example. The results indicated that the evolution of the ceramic and metallic phases in the cermet particle during the heating, melting and solidification processes were all significantly inhomogeneous from atomic scale to mesoscale microstructures. As a consequence, the microstructural defects were caused intrinsically in the printed bulk material. The formation and growth of the bonding necks between the particles were mainly completed at the later stage of laser heating and the early stage of solidification. Both simulations and experiments demonstrated that thin amorphous layers formed at the ceramics/metal interfaces. This work disclosed the mechanisms for the evolution from the atomic scale to microstructure during the SLM printing of cermet powders, and discovered the origin of the defects in the printed cermet bulk materials. 相似文献
9.
《International Journal of Hydrogen Energy》2022,47(4):2279-2292
A new catalyst for both water reduction and oxidation, based on an infinite chain, {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n, is formed by the reaction of NiCl2, 1,3-propanediamine (tn) and K3 [Fe(CN)6]. {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n can electro-catalyze hydrogen evolution from a neutral aqueous buffer (pH 7.0) with a turnover frequency (TOF) of 1561 mol of hydrogen per mole of catalyst per hour (H2/mol catalyst/h) at an overpotential (OP) of 837 mV {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n also can electro-catalyze O2 production from water with a TOF of ~45 mol O2 (mol cat)?1s?1 at an OP of 591 mV. Under blue light (λ = 469 nm), together with CdS nanorods (CdS NRs) as a photosensitizer, and ascorbic acid (H2A) as a sacrificial electron donor, {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n can photo-catalyze hydrogen generation from an aqueous buffer (pH 4.0) with a turnover number (TON) of 11,450 mol H2 per mole of catalyst (mol of H2 (mol of cat)?1) during 10 h irradiation. The average of apparent quantum yield (AQY) is as high as 40.96% during 10 h irradiation. Studies indicate that {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n exists in two forms: a cyano-bridged chain ({[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n) in solid, and a salt ([Ni(tn)2]3 [Fe(CN)6]2) in aqueous media; Catalytic reaction occurs on the nickel center of [Ni(tn)2]2+, and the introduction of [Fe(CN)6]3- can improve the catalytic efficiency of [Ni(tn)2]2+ for H2 or O2 generation. We hope these findings can afford a new method for the design of catalysts for both water reduction and oxidation. 相似文献
10.
《International Journal of Hydrogen Energy》2022,47(54):22981-22992
In this study, a three-dimensional model was established using the lattice Boltzmann method (LBM) to study the internal ice melting process of the gas diffusion layer (GDL) of the proton exchange membrane fuel cell (PEMFC). The single-point second-order curved boundary condition was adopted. The effects of GDL carbon fiber number, growth slope of the number of carbon fibers and carbon fiber diameter on ice melting were studied. The results were revealed that the temperature in the middle and lower part of the gradient distribution GDL is significantly higher than that of the no-gradient GDL. With the increase of the growth slope of the number of carbon fiber, the temperature and melting rate gradually increase, and the position of the solid-liquid interface gradually decreases. The decrease in the number of carbon fibers has a similar effect as the increase in the growth slope of the number of carbon fibers. In addition, as the diameter of the carbon fiber increases, the position of the solid-liquid interface gradually decreases first and then increases. 相似文献