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Bimetallic nanoparticles with tailored structures constitute a desirable model system for catalysts, as crucial factors such as geometric and electronic effects can be readily controlled by tailoring the structure and alloy bonding of the catalytic site. Here we report a facile colloidal method to prepare a series of platinum–gold (PtAu) nanoparticles with tailored surface structures and particle diameters on the order of 7 nm. Samples with low Pt content, particularly Pt4Au96, exhibited unprecedented electrocatalytic activity for the oxidation of formic acid. A high forward current density of 3.77 A mgPt−1 was observed for Pt4Au96, a value two orders of magnitude greater than those observed for core–shell structured Pt78Au22 and a commercial Pt nanocatalyst. Extensive structural characterization and theoretical density functional theory simulations of the best-performing catalysts revealed densely packed single-atom Pt surface sites surrounded by Au atoms, which suggests that their superior catalytic activity and selectivity could be attributed to the unique structural and alloy-bonding properties of these single-atomic-site catalysts.

HighlightsCatalytically inert 2D Bi2O3 is activated for boosting electrochemical hydrogen evolution reaction (HER) via oxygen vacancy concentration modulation.The relationship between the varied oxygen vacancy concentrations and the corresponding HER activity is revealed by both experimental Vo verification and theoretical density-functional theory calculations.This work provides insights into activating catalytically inert materials into high-performance catalysts.Oxygen vacancies (Vo) in electrocatalysts are closely correlated with the hydrogen evolution reaction (HER) activity. The role of vacancy defects and the effect of their concentration, however, yet remains unclear. Herein, Bi2O3, an unfavorable electrocatalyst for the HER due to a less than ideal hydrogen adsorption Gibbs free energy (ΔGH*), is utilized as a perfect model to explore the function of Vo on HER performance. Through a facile plasma irradiation strategy, Bi2O3 nanosheets with different Vo concentrations are fabricated to evaluate the influence of defects on the HER process. Unexpectedly, while the generated oxygen vacancies contribute to the enhanced HER performance, higher Vo concentrations beyond a saturation value result in a significant drop in HER activity. By tunning the Vo concentration in the Bi2O3 nanosheets via adjusting the treatment time, the Bi2O3 catalyst with an optimized oxygen vacancy concentration and detectable charge carrier concentration of 1.52 × 1024 cm−3 demonstrates enhanced HER performance with an overpotential of 174.2 mV to reach 10 mA cm−2, a Tafel slope of 80 mV dec−1, and an exchange current density of 316 mA cm−2 in an alkaline solution, which approaches the top-tier activity among Bi-based HER electrocatalysts. Density-functional theory calculations confirm the preferred adsorption of H* onto Bi2O3 as a function of oxygen chemical potential (∆μO) and oxygen partial potential (PO2) and reveal that high Vo concentrations result in excessive stability of adsorbed hydrogen and hence the inferior HER activity. This study reveals the oxygen vacancy concentration-HER catalytic activity relationship and provides insights into activating catalytically inert materials into highly efficient electrocatalysts.

Selective laser melting (SLM) additive manufacturing of pure tungsten encounters nearly all intractable difficulties of SLM metals fields due to its intrinsic properties. The key factors, including powder characteristics, layer thickness, and laser parameters of SLM high density tungsten are elucidated and discussed in detail. The main parameters were designed from theoretical calculations prior to the SLM process and experimentally optimized. Pure tungsten products with a density of 19.01 g/cm 3 (98.50% theoretical density) were produced using SLM with the optimized processing parameters. A high density microstructure is formed without significant balling or macrocracks. The formation mechanisms for pores and the densification behaviors are systematically elucidated. Electron backscattered diffraction analysis confirms that the columnar grains stretch across several layers and parallel to the maximum temperature gradient, which can ensure good bonding between the layers. The mechanical properties of the SLM-produced tungsten are comparable to that produced by the conventional fabrication methods, with hardness values exceeding 460 HV 0.05 and an ultimate compressive strength of about 1 GPa. This finding offers new potential applications of refractory metals in additive manufacturing.

In this work, two different types of ZnAl-layered double hydroxide (LDH) mixed metal-oxide composites (CeO 2 and SnO 2 ) were synthesized and applied for the photodegradation of 4-chlorophenol (4-CP) in wastewater. The fabricated CeO 2 /ZnAl-LDH and SnO 2 /ZnAl-LDH were characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, UV–visible diffuse reflectance spectroscopy (UV–vis DRS), and theoretical density functional theory (DFT) calculations, suggesting that the band gaps of the synthesized hybrid composites were much lower than those of traditional ZnAl-LDH. In addition, the photocatalytic activity for 4-CP degradation and reaction kinetics were investigated to evaluate the catalytic behavior of the prepared composites. The results indicated that the photocatalytic process in this case followed a pseudo-first-order kinetic model, and SnO 2 /ZnAl-LDH illustrated the optimum performance for 4-CP degradation with an efficiency of 95.2% due to its stability and recyclability. Additionally, the reaction mechanism of 4-CP photodegradation was studied over SnO 2 /ZnAl-LDH; it presented that 4-CP could be oxidized by hydroxyl radicals, holes, and superoxide radicals, where hydroxyl radicals were identified as the dominant active species during the degradation process. Finally, decomposition intermediates were measured to deduce the reaction pathway of 4-CP, and three tentative pathways were proposed and discussed.

Hexagonal boron nitride (hBN) ceramics are expected to have wide applications at high temperatures as both a structural and functional material. However, because of its flake structure and general inertness, it is currently impossible to sinter hBN powder to a dense bulk (with a relative density of above 96%) even at 2000 °C. Here, we report dense bulk hBN with 97.6% theoretical density achieved at a lower preparation temperature (1700 °C) via a self-densifying mechanism without sintering additives. During the sintering process, cubic boron nitride particles incorporated into the hBN flake powders transform into BN onions with a significant volume increase, thus filling in voids among the hBN flakes and highly densifying the hBN bulks. The resulting dense hBN ceramics possess 2–3 times the strength of traditional hBN ceramics. This phase-transition-induced volume expansion strategy could lead to dense sintered compacts with high performance in other ceramic systems. Sintering hexagonal boron nitride until it is more than 96% dense remains a challenge. Here, the authors mix cubic boron nitride particles into hexagonal boron nitride flakes and sinter the combined powders to obtain dense hexagonal boron nitride ceramics with significantly increased strength.

Advanced ceramic materials with complex design have become inseparable from the current engineering applications. Due to the limitation of traditional ceramic processing, ceramic additive manufacturing (AM) which allows high degree of fabrication freedom has gained significant research interest. Among these AM techniques, low-cost robocasting technique is often considered to fabricate complex ceramic components. In this work, aqueous ceramic suspension comprising of commercial nano-sized yttria-stabilized zirconia (YSZ) powder has been developed for robocasting purpose. Both fully and partially stabilized YSZ green bodies with complex morphologies were successfully printed in ambient conditions using relatively low-solid-content ceramic suspensions (<38 vol%). The sintered structures were able to retain the original morphologies with >94% of the theoretical density despite its high linear shrinkage (up to 33%). The microstructure analysis indicated that dense fully and partially stabilized YSZ with grain size as small as 1.40 ± 0.53 and 0.38 ± 0.10 μm can be obtained, respectively. The sintered partially stabilized YSZ solid and porous mesh samples (porosity of macro-pores >45%) exhibited hardness up to 13.29 GPa and flexural strengths up to 242.8 ± 11.4 and 57.3 ± 5.2 MPa, respectively. The aqueous-based ceramic suspension was also demonstrated to be suitable for the fabrication of large YSZ parts with good repeatability.

This paper presents an experimental study on the influence of the main Laser Powder Bed Fusion (PBF-LB) process parameters on the density and surface quality of the IN 625 superalloy manufactured using the Lasertec 30 SLM machine. Parameters’ influence was investigated within a workspace defined by the laser power (150–400 W), scanning speed (500–900 m/s), scanning strategy (90° and 67°), layer thickness (30–70 µm), and hatch distance (0.09–0.12 µm). Experimental results showed that laser power and scanning speed play a determining role in producing a relative density higher than 99.5% of the material’s theoretical density. A basic set of process parameters was selected for generating high-density material: laser power 250 W, laser speed 750 mm/s, layer thickness 40 µm, and hatch distance 0.11 mm. The 67° scanning strategy ensures higher roughness surfaces than the 90° scanning strategy, roughness that increases as the laser power increases and the laser speed decreases.

Context High-energy density materials (HEDMs) are integral to modern society and are in high demand. Consequently, the design and synthesis of energetic material molecules have garnered significant research interest. This study focuses on the furazan ring system as a core for developing superior HEDMs. We employed density functional theory (DFT) to assess the properties of 27 novel energetic compounds, including their geometries, densities, enthalpies of formation, detonation velocities, detonation pressures, and molecular orbital energies (HOMO–LUMO). The computation of detonation velocity and detonation pressure was based on theoretical density and enthalpy of formation. The findings revealed that incorporating energetic groups into the furazan framework, linked by sec-ammonia bridge (-NH-), enhances both the detonation performance and oxygen content of the materials. This enhancement guides the future synthetic endeavors aimed at creating advanced HEDMs. Method DFT has been employed to investigate the detonation performance and stability of energetic materials. Molecular optimization and performance metrics were all calculated using the DFT-B3LYP method with a 6–311 + G* basis set. The optimization and volume calculations were performed using the Gaussian 09 package. The electrostatic potential energy was computed using Multiwfn software. The impact sensitivity of the designed molecules was calculated using the heat of detonation model.

High-entropy boride-silicon carbide (HEB-SiC) ceramics were fabricated using boride-based powders prepared from borothermal and boro/carbothermal reduction methods. The effects of processing routes (borothermal reduction and boro/carbothermal reduction) on the HEB powders were examined. HEB-SiC ceramics with > 98% theoretical density were prepared by spark plasma sintering at 2000 °C. It was demonstrated that the addition of SiC led to slight coarsening of the microstructure. The HEB-SiC ceramics prepared from boro/carbothermal reduction powders showed a fine-grained microstructure and higher Vickers’ hardness but lower fracture toughness value as compared with the same composition prepared from borothermal reduction powders. These results indicated that the selection of the powder processing method and the addition of SiC phase could contribute to the optimal preparation of high-entropy boride-based ceramics.

The aim of this article is to explore the dynamic compaction characteristics of stone mastic asphalt (SMA) and the friction–lubrication effect of internal particles during the superpave gyratory compaction (SGC) process. Firstly, a calculated method for the compaction degree of an asphalt mixture in the gyratory compaction process was defined based on the multiphase granular volume method. Secondly, the gyratory compaction curves of asphalt mixtures were taken based on this calculation method of compaction degree. The dynamic change law of each compaction index (compaction, percentage of air voids, compaction energy index, etc.) during the compaction process was analysed. Finally, the effects of different initial compaction temperatures and different asphalt content on the friction–lubrication effect and compaction characteristics of asphalt mixtures were studied. Research shows that it is reasonable to define the compaction degree by the ratio of the apparent density of the asphalt mixture to the maximum theoretical density of the asphalt mixture during gyratory compaction. The dynamic prediction equations of the compaction degree K and the compaction energy index CEI with the amount of compaction were established, and could effectively predict the compaction degree, percentage of air voids and compaction energy index CEI. The compaction process of the asphalt mixture needed to go through three phases, including periods of rapid growth, slow growth, and stabilisation, and the compaction degree increased by about 10%, 5%, and 1%, in that order, finally tending towards a stable value. The effect of the initial compaction temperature on the forming compaction degree of the asphalt mixture is significant; therefore, it should be controlled strictly in the compaction construction of asphalt mixtures. When the initial compaction temperature of SMA-13 is about 170 °C, the compaction effect is optimal, and the effect of the increase in the amount of compaction at a later stage on the increase in the compaction degree of the asphalt mixture is very low. With the optimal asphalt content, the friction–lubrication effect between the asphalt and aggregate particles is optimal, because it can effectively form an asphalt film, reducing the frictional resistance of the particles moving each other during the compaction process, and the voids will be embedded and filled with each other, finally producing the best compaction result.