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A coating made of platinum-gold alloy is provided, together with a method of its preparation by electrodeposition. The alloy is composed of more than 50 atomic percent platinum. The microstructure of the alloy consists of generally ellipsoidal grains. More than half of the grains have a major axis of 10 nm or less.
The valence electronic structures of the dental gold alloys, type 1, type 3, and K14, and their interaction with L-cysteine have been studied by ultraviolet photoelectron spectroscopy with synchrotron radiation. It was found that the electronic structures of the type-1 and type-3 dental alloys are similar to that of polycrystalline Au, while that of the K14 dental alloy is much affected by Cu. The peak shift and the change in shape due to alloying are observed in all the dental alloys. It is suggested that the new peak observed around 2 eV for the L-cysteine thin films on all the dental alloys may be due to the bonding of S 3sp orbitals with the dental alloy surfaces, and the Cu-S bond, as well as the Au-S and Au-O bonds, may cause the change in the electronic structure of the L-cysteine on the alloys.
Abstract The ability to control phase structures and surface sites of ultrasmall alloy nanoparticles under reaction conditions is essential for preparing catalysts by design. This is, however, challenging due to limited understanding of the atomic‐scale phases and their correlation with the ensemble‐averaged structures and activities of catalysts during catalytic reactions. We reveal here a dynamic structural stability of alumina‐supported ultrasmall and equiatomic copper‐gold alloy nanoparticles under reaction conditions as a model system in the in situ/operando study. In situ atomic‐scale morphological tracking under oxygen reveals temperature‐dependent dynamic crystalline‐amorphous dual‐phase structures, showing dynamic stability over an elevated temperature range. This atomic‐scale dynamic phase stability coincides with a “conversion plateau” observed for carbon monoxide oxidation on the catalyst. It is substantiated by the stable lattice ordering/disordering structures and surface sites with oscillatory characteristics shown by operando ensemble‐average structural tracking of the catalyst during the oxidation reaction. The understanding of the atomic‐scale dynamic phase structures in correlation with the ensemble‐average dynamic ordering/disordering phase structures and surface sites provides fresh insights into the unique synergy of the supported alloy nanoparticles. This understanding has implications for the design and structural tuning of active and stable ultrasmall alloy catalysts under elevated temperatures.
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Bimetallic, nanostructured materials hold promise for improving catalyst activity and selectivity, yet little is known about the dynamic compositional and structural changes that these systems undergo during pretreatment that leads to efficient catalyst function. Here we use ozone-activated silver–gold alloys in the form of nanoporous gold as a case study to demonstrate the dynamic behaviour of bimetallic systems during activation to produce a functioning catalyst. We show that it is these dynamic changes that give rise to the observed catalytic activity. Advanced in situ electron microscopy and X-ray photoelectron spectroscopy are used to demonstrate that major restructuring and compositional changes occur along the path to catalytic function for selective alcohol oxidation. Transient kinetic measurements correlate the restructuring to three types of oxygen on the surface. The direct influence of changes in surface silver concentration and restructuring at the nanoscale on oxidation activity is demonstrated. Finally, our results demonstrate that characterization of these dynamic changes is necessary to unlock the full potential of bimetallic catalytic materials.
Gold-tantalum alloy films are of interest for biomedical and magnetically-assisted inertial confinement fusion applications. Here, we systematically study the effects of substrate tilt (0°–80°) and negative substrate bias (0–100 V) on properties of ≲3-μm-thick films deposited by high-power impulse magnetron sputtering (HiPIMS) from a Au–Ta alloy target (with 80 at. % of Ta). Results reveal that, for all the substrate bias values studied, an increase in substrate tilt leads to a monotonic decrease in film thickness, density, residual compressive stress, and electrical conductivity. Larger substrate bias favors the formation of a body-centered cubic phase, with films exhibiting lower column tilt and higher density, electrical conductivity, and residual compressive stress. Furthermore, these changes are attributed to metal atom ionization effects, based on the lack of correlation with distributions of landing energies and incident angles of depositing species as calculated by Monte Carlo simulations of ballistic collisions and gas phase atomic transport. By varying substrate tilt and bias in HiPIMS deposition, properties of Au–Ta alloy films can be controlled in a very wide range, including residual stress from –2 to +0.5 GPa, density from 12 to 17 g/cm 3 , and the electrical resistivity from 50 to 4500 μΩ cm, enabling optimum deposition conditions to be selected for specific applications.
Abstract—: Nanowires are one of the most promising building blocks for various nanoelectronic devices. Nanowires are usually grown via the so-called vapor-liquid-solid mechanism on the surfaces activated by the droplets of a catalyst (e.g., Au). Here we theoretically studied the impact of the evaporation from the droplet on the nucleation statistics. Within the semi-analyticalapproach, we obtain the relation between the nucleation time distributions and the evaporation rate of atoms from the droplet. We analyze the Si NW length-time dependences to estimate theeffective lifetime of a silicon atom in a gold-silicon alloy at 550°C is about 5 s.
The unique yet tunable optical properties of plasmonic metal nanoparticles have made them attractive targets for a wide range of applications including nanophotonics, molecular sensing, catalysis etc. Such diverse applications that require precisely stable / reproducible plasmonic properties depend sensitively on the particle morphology ie. the shape, size and constituents. Herein, we systematically study the size / shape controlled synthesis of gold-copper “dumpling” shaped alloy nanoparticles by simultaneous reduction of gold and copper salts in the PVP-methanol solute-solvent system, by effectively utilizing the efficient but mild reduction as well as capping abilities of Poly (N-vinylpyrrolidone). Introduction of copper salts not only yielded the alloy nanoparticles, but also slowed down the growth process to maintain high mono-dispersity of the new shapes evolved. Copper and gold has different lattice constants (0.361 and 0.408 nm respectively) and hence doping/addition/replacement of copper atoms to gold FCC unit cell introduces strain into the lattice which is key parameter to the shape evolution in anisotropic nanoparticles. Synthesized alloy nanoparticles were characterized by UV-visible absorption spectroscopy, XRD and TEM imaging.
For Inertial Confinement Fusion (ICF) implosions, a design based on gradients of high and mid Z materials could potentially be more robust than single element capsule systems. To that end, gold and silver alloys were electroplated on 2.0 mm diameter surrogate brass spheres using a new flow–based pulsed plating method specifically designed to minimize surface roughness without reducing plating rates. The coatings were analyzed by scanning electron microscope (SEM) and white light interferometry for surface topography, and by energy dispersive x-ray spectroscopy (EDX) to determine near-surface gold and silver compositions. The alloy range attainable was 15 to 85 weight percent gold using 1:1 and 1:3 silver to gold ratio plating baths at applied potentials of -0.7 volts to -1.8 volts. This range was bounded by the open circuit potential of the system and hydrogen evolution, and in theory could be extended by using ionic liquids or aprotic solutions. Preliminary gradient trials proved constant composition alloy data could be translated to smooth gradient plating, albeit at higher gold compositions.
Earlier detection of breast cancer reduces mortality from this disease. Thus, the development of better screening techniques is a topic of intense interest. Contrast-enhanced dual-energy mammography (DEM) is a novel technique that has improved sensitivity for cancer detection. However, the development of contrast agents for this technique is in its infancy. We herein report gold-silver alloy nanoparticles (GSAN) that have potent DEM contrast properties and improved biocompatibility. GSAN formulations containing a range of gold:silver ratios and capped with m-PEG were synthesized and characterized using various analytical methods. DEM and computed tomography (CT) phantom imaging showed that GSAN produced robust contrast that was comparable to silver alone. Cell viability, reactive oxygen species generation and DNA damage results revealed that the formulations with 30% or higher gold content are cytocompatible to Hep G2 and J774A.1 cells. In vivo imaging was performed in mice with and without breast tumors. The results showed that GSAN produce strong DEM and CT contrast and accumulated in tumors. Furthermore, both in vivo imaging and ex vivo analysis indicated the excretion of GSAN via both urine and feces. In summary, GSAN produce strong DEM and CT contrast, and has potential for both blood pool imaging and for breast cancer screening.
This paper reports the development of fiber optical hydrogen sensors using palladium and gold alloy nanostructures as sensor materials for hydrogen measurements using a D-shaped fiber as a platform. Using a maskless reactive ion etching technique, silica nanocone structures were formed on the surface of the D-shaped fiber. Palladium and gold alloys were deposited on the surface of nanostructured D-shaped fiber to form a nano-alloy sensor film. Evanescent interaction between guided light propagated in the fiber core and nano-alloy enabled highly sensitive hydrogen detection from concentrations that ranged from 0.25% to 10% in atmosphere pressure. Here, the formation of nanostructured alloy enabled by the nanocone surface led to more than 3 times faster in sensor response time and significant improvements in sensor sensitivity and reversibility. The work presented here demonstrates that highly controllable VLSI microfabrication schemes can be applied to produce nanostructured sensor films on optical fibers for high-sensitivity chemical sensing.
Dilute palladium-in-gold alloys have potential as efficient oxidation catalysts; controlling the Pd surface distribution is critical.
Understanding the catalytic oxidation of propane is important for developing catalysts not only for catalytic oxidation of hydrocarbons in emission systems but also for selective oxidation in the chemical processing industry. For palladium-based catalysts, little is known about the identification of the chemical or intermediate species involved in propane oxidation. We describe herein findings of an investigation of the catalytic oxidation of propane over supported palladium nanoalloys with different compositions of gold (Pd n Au 100–n ), focusing on probing the chemical or intermediate species on the catalysts in correlation with the bimetallic composition and the alloying phase structure. In addition to an enhanced catalytic activity, a strong dependence of the catalytic activity on the bimetallic composition was revealed, displaying an activity maximum at a Pd : Au ratio of 50 : 50 in terms of reaction temperature. This dependence is also reflected by its dependence on the thermochemical treatment conditions. While the activity for nanoalloys with n ~ 50 showed little change after the thermochemical treatment under oxygen, the activities for nanoalloys with n < 50 and n > 50 showed opposite trends. Importantly, this catalytic synergy is linked to the subtle differences of chemical and intermediate species which have been identified for the catalysts with different bimetallic compositions by in situ measurements using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). For the catalytic oxidation of propane over the highly-active catalyst with a Pd : Au ratio of 50 : 50, the major species identified include acetate and bicarbonate, showing subtle differences in comparison with the identification of bicarbonate and formate for the catalyst with <50% Au (with a lower activity) and the absence of apparent species for the catalyst with >50% Au (activity is largely absent). The alloying of 50% Au in Pd is believed to increase the oxophilicity of Pd, which facilitates the first carbon–carbon bond cleavage and oxygenation of propane. Finally, the implications of the findings on the catalytic synergy of Pd alloyed with Au and the design of active Pd alloy catalysts are also discussed.
Purpose: High-density materials used in dental restoration can cause significant localized dose enhancement due to electron backscatter in head-and-neck radiotherapy, increasing the risk of mucositis. The materials used in prosthetic dentistry have evolved in the last decades from metal alloys to ceramics. We aim to determine the dose enhancement caused by backscatter from currently-used dental materials. Methods: Measurements were performed for three different dental materials: lithium disilicate (Li{sub 2}Si{sub 2}O{sub 5}), zirconium dioxide (ZrO{sub 2}), and gold alloy. Small thin squares (2×2×0.15 cm{sup 3}) of the material were fabricated, and placed into a phantom composed of tissue-equivalent material. The phantom was irradiated with a single 6 MV photon field. A thin-window parallel-plate ion chamber was used to measure the dose at varying distances from the proximal interface between the material and the plastic. Results: The dose enhancement at the interface between the high-density and tissue-equivalent materials, relative to a homogeneous phantom, was 54% for the gold alloy, 31% for ZrO{sub 2}, and 9% for Li{sub 2}Si{sub 2}O{sub 5}. This enhancement decreased rapidly with distance from the interface, falling to 11%, 5%, and 0.5%, respectively, 2 mm from the interface. Comparisons with the modeling of this effect in treatment planning systems are performed. Conclusion: While dose enhancement due to dental restoration is smaller with ceramic materials than with metal alloys, it can still be significant. A spacer of about 2–3 mm would be effective in reducing this enhancement, even for metal alloys.
Solute segregation to grain boundaries in polycrystalline metals and ceramics is a well-known phenomenon that reduces the total energy of the material. In this letter, the segregation of the solvent (Au) to grain boundaries in a binary Au 1-x Pt x (x = 0.15 to 0.18) alloy is demonstrated. After heating in the range of 500 °C to 600 °C and quenching to room temperature, grain boundaries in the alloy are enriched in Au at a mean level of ∼ 4 atoms/nm 2 . When the alloy is annealed at 300 °C and quenched, the mean grain boundary composition is closer to the bulk composition. When the alloy is reheated to 500 °C, the segregation is reestablished, demonstrating that the transformation from the strongly segregated complexion to the weakly segregated complexion is reversible. The driving force for the solvent segregation is likely the lower grain boundary energy of Au in comparison to Pt.