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At least 991 records · Page 55
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Catalysis applications of size-selected cluster deposition

In this Perspective, we review recent studies of size-selected cluster deposition for catalysis applications performed at the U.S. DOE National Laboratories, with emphasis on work at Argonne National Laboratory (ANL) and Brookhaven National Laboratory (BNL). The focus is on the preparation of model supported catalysts in which the number of atoms in the deposited clusters is precisely controlled using a combination of gas-phase cluster ion sources, mass spectrometry, and soft-landing techniques. This approach is particularly effective for investigations of small nanoclusters, 0.5-2 nm (<200 atoms), where the rapid evolution of the atomic and electronic structure makes it essential to have precise control over cluster size. Cluster deposition allows for independent control of cluster size, coverage, and stoichiometry (e.g., the metal-to-oxygen ratio in an oxide cluster) and can be used to deposit on any substrate without constraints of nucleation and growth. Examples are presented for metal, metal oxide, and metal sulfide cluster deposition on a variety of supports (metals, oxides, carbon/diamond) where the reactivity, cluster-support electronic interactions, and cluster stability and morphology are investigated. Both UHV and in situ/operando studies are presented that also make use of surface-sensitive X-ray characterization tools from synchrotron radiation facilities. Novel applications of cluster deposition to electrochemistry and batteries are also presented. This review also highlights the application of modern ab initio electronic structure calculations (density functional theory), which can essentially model the exact experimental system used in the laboratory (i.e., cluster and support) to provide insight on atomic and electronic structure, reaction energetics, and mechanisms. As amply demonstrated in this review, the powerful combination of atomically precise cluster deposition and theory is able to address fundamental aspects of size-effects, cluster-support interactions, and reaction mechanisms of cluster materials that are central to how catalysts function. Lastly, the insight gained from such studies can be used to further the development of novel nanostructured catalysts with high activity and selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition

Reactive uptake of isoprene epoxydiols (IEPOX), which are isoprene oxidation products, onto acidic sulfate aerosols is recognized to be an important mechanism for the formation of isoprene-derived secondary organic aerosol (SOA). While a mechanistic understanding of IEPOX-SOA formation exists, several processes affecting their formation remain uncertain. Evaluating mechanistic IEPOX-SOA models with controlled laboratory experiments under longer atmospherically relevant timescales is critical. Here, we implement our latest understanding of IEPOX-SOA formation within a box model to simulate the measured reactive uptake of IEPOX on polydisperse ammonium bisulfate seed aerosols within an environmental Teflon chamber. The model is evaluated with single-particle measurements of size distribution, volume, density, and composition of aerosols due to IEPOX-SOA formation at timescales of hours. Additionally, we find that the model can simulate the growth of particles due to IEPOX multiphase chemistry, as reflected in increases of the mean particle size and volume concentrations, and a shift of number size distribution to larger sizes. The model also predicts the observed evolution of particle number mean diameter and total volume concentrations at the end of the experiment. We show that in addition to self-limiting effects of IEPOX-SOA coatings, accounting for the molar balance between inorganic and organic sulfate and mass accommodation coefficient of IEPOX are important parameters governing modeling of IEPOX-SOA formation. Thus, models which do not account for the molar sulfate balance and/or diffusion limitations within IEPOX-SOA coatings are likely to predict too high IEPOX-SOA formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Excitation Intensity- and Size-Dependent Halide Photosegregation in CsPb(I 0.5 Br 0.5 ) 3 Perovskite Nanocrystals

Although broad consensus exists that photoirradiation of mixed-halide lead perovskites leads to anion segregation, no model today fully rationalizes all aspects of this near ubiquitous phenomenon. In this work, we quantitatively compare experimental, CsPb(I 0.5 Br 0.5 ) 3 nanocrystal (NC) terminal anion photosegregation stoichiometries and excitation intensity thresholds to a band gap-based, thermodynamic model of mixed-halide perovskite photosegregation. Mixed-halide NCs offer strict tests of theory given physical sizes, which dictate local photogenerated carrier densities. We observe that mixed-anion perovskite NCs exhibit significant robustness to photosegregation, with photosegregation propensity decreasing with decreasing NC size. Observed size- and excitation intensity-dependent photosegregation data agree with model predicted size- and excitation intensity-dependent terminal halide stoichiometries. Established correspondence between experiment and theory, in turn, suggests that mixed-halide perovskite photostabilities can be predicted a priori using local gradients of (empirical) Vegard’s law expressions of composition-dependent band gaps.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Effect of particle size on the thermo-optic properties of gold nanofluids – A thermal lens study

Spherical gold nanoparticles having particle size in the range 30 to 50 nm are prepared using citrate reduction of gold chloride trihydrate in water. The influence of particle size on the thermal diffusivity value of gold nanofluid is measured using dual beam thermal lens technique. The present study shows that the particle size influences the effective thermal diffusivity value of the nanofluid substantially and the value decreases with decrease in particle size for the investigated samples.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Annealing effect on the particle size and chemical composition of activated carbon obtained from vacuum furnace of teak sawdust

Activated carbon was produced from sawdust by using physical method in a high temperature vacuum furnace without additional chemical. Fast pyrolysis process was carried out prior in fluidized a bed furnace to produce char before activation process. Experiments were conducted to investigate the influence of various process parameters such as particle size, activation temperature and activation time on the quality of the activated carbon. In addition, the chemical composition studies were done by using x-ray fluorescence (XRF) spectroscopy. The crystallite sizes were calculated by using Scherer equation based on x-ray diffraction (XRD) spectroscopy data. The pyrolysis temperature and time were varied from 600°C to 900°C and from 3 hours to 6 hours, respectively. The particle size of activated carbon was increase with increasing temperature. The composition and crystallite size of the prepared activated carbon was compared with the non-activated carbon. The results indicated that the teak sawdust carbon could be employed as a low cost alternative to produce commercial activated carbon.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Size effect of strong-coupled superconducting In{sub 2}Bi nanoparticles: An investigation of short-range electron phonon coupling

We report the influence of the nanosized effect on the superconducting properties of bimetallic In{sub 2}Bi nanoparticles. In this study, the temperature- and applied magnetic field-dependence of the magnetization were utilized to investigate the electron-phonon coupling effect while controlling particle sizes 〈d〉 from 21(2) to 42(5) nm. As the particle size decreases, the electron-phonon constant λ{sub EP} decreases rapidly, signaling the short-range electron-phonon coupling effect which acts to confine the electrons within a smaller volume, thereby giving rise to a higher superconducting transition temperature T{sub C}. An enhanced superconducting transition was observed from the temperature dependence of magnetization, revealing a main diamagnetic Meissner state below T{sub C} ∼ 5.72(5) K for 〈d〉 = 31(1) nm In{sub 2}Bi nanoparticles. The variation of the T{sub C} is very sensitive to the particle size, which might be due to crystallinity and size uniformity of the samples. The electron-phonon coupling to low lying phonons is found to be the leading mechanism for the observed strong-coupling superconductivity in the In{sub 2}Bi system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

The effect of particle size on the morphology and thermodynamics of diblock copolymer/tethered-particle membranes

A combination of self-consistent field theory and density functional theory was used to examine the effect of particle size on the stable, 3-dimensional equilibrium morphologies formed by diblock copolymers with a tethered nanoparticle attached either between the two blocks or at the end of one of the blocks. Particle size was varied between one and four tenths of the radius of gyration of the diblock polymer chain for neutral particles as well as those either favoring or disfavoring segments of the copolymer blocks. Phase diagrams were constructed and analyzed in terms of thermodynamic diagrams to understand the physics associated with the molecular-level self-assembly processes. Typical morphologies were observed, such as lamellar, spheroidal, cylindrical, gyroidal, and perforated lamellar, with the primary concentration region of the tethered particles being influenced heavily by particle size and tethering location, strength of the particle-segment energetic interactions, chain length, and copolymer radius of gyration. The effect of the simulation box size on the observed morphology and system thermodynamics was also investigated, indicating possible effects of confinement upon the system self-assembly processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Parametric interactions in presence of different size colloids in semiconductor quantum plasmas

Present work is an attempt to investigate the effect of different size colloids on parametric interaction in semiconductor quantum plasma. Inclusion of quantum effect is being done in this analysis through quantum correction term in classical hydrodynamic model of homogeneous semiconductor plasma. The effect is associated with purely quantum origin using quantum Bohm potential and quantum statistics. Colloidal size and quantum correction term modify the parametric dispersion characteristics of ion implanted semiconductor plasma medium. It is found that quantum effect on colloids is inversely proportional to their size. Moreover critical size of implanted colloids for the effective quantum correction is determined which is found to be equal to the lattice spacing of the crystal.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Ultrafast image-based dynamic light scattering for nanoparticle sizing

An ultrafast sizing method for nanoparticles is proposed, called as UIDLS (Ultrafast Image-based Dynamic Light Scattering). This method makes use of the intensity fluctuation of scattered light from nanoparticles in Brownian motion, which is similar to the conventional DLS method. The difference in the experimental system is that the scattered light by nanoparticles is received by an image sensor instead of a photomultiplier tube. A novel data processing algorithm is proposed to directly get correlation coefficient between two images at a certain time interval (from microseconds to milliseconds) by employing a two-dimensional image correlation algorithm. This coefficient has been proved to be a monotonic function of the particle diameter. Samples of standard latex particles (79/100/352/482/948 nm) were measured for validation of the proposed method. The measurement accuracy of higher than 90% was found with standard deviations less than 3%. A sample of nanosilver particle with nominal size of 20 ± 2 nm and a sample of polymethyl methacrylate emulsion with unknown size were also tested using UIDLS method. The measured results were 23.2 ± 3.0 nm and 246.1 ± 6.3 nm, respectively, which is substantially consistent with the transmission electron microscope results. Since the time for acquisition of two successive images has been reduced to less than 1 ms and the data processing time in about 10 ms, the total measuring time can be dramatically reduced from hundreds seconds to tens of milliseconds, which provides the potential for real-time and in situ nanoparticle sizing.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Synthesis of nano-sized ZnO particles by co-precipitation method with variation of heating time

Zinc oxide powders have been synthesized by a co-precipitation method at low temperature (85 °C), using zinc acetate dihydrate, ammonia, hydrochloric acid solutions as the reactants. A number of process parameters such as reaction temperature, solution basicity or pH and heating time are the main factors affecting the morphology and physical properties of the ZnO nanostructures. In this work the effect of heating time on the morphology and particles size were studied. The as-synthesized ZnO powders were characterized using transmission electron microscopy (TEM) and X-ray diffraction (XRD) techniques. The samples were also analyzed using Fourier transform infrared (FTIR). Rietveld refinement of XRD data confirms that ZnO crystallizes in the hexagonal wurtzite structure with high degree of purity and the (101) plane predominant. The XRD results show that the average crystallite sizes were about 66, 27 and 12 nm for 3, 4 and 5 h of heating times, respectively. The XRD analysis indicated that a fraction of nano-sized ZnO powders were in the form of aggregates, which was also verified by TEM image. The TEM photograph demonstrated that the nano-sized ZnO particles were a pseudo-spherical shape.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Structure and particle size analysis of LaFeO{sub 3} nanoparticles

Particle size analysis of LaFeO{sub 3} nanoparticles has been done through different methods. A simple low temperature syntheses of LaFeO{sub 3}-NPs were carried out via PVA based sol-gel method. The role of PVA in this method is complexing agent. The product were characterized with the help of X-ray diffraction (XRD), Field Emission Scanning Electron Microscopy (FE-SEM), and Transmission Electron Microscopy (TEM). The Rietveld refinement on X-ray diffraction peaks have been done in order to calculate various structural parameters. The Scherrer method was applied to calculate the crystallite size. Further, the crystallite size and associated lattice strain of LaFeO{sub 3}-NPs were studied using Williamson-Hallmethod. The FESEM image shows the presence of spherical morphology. The formation of LaFeO{sub 3} nanoscale particles, with their size, has been confirmed by TEM characterization.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

The effect of dogbone sample size in the tensile testing of TATB-based plastic‑bonded explosive materials

Mechanical properties are of interest for many plastic‑bonded explosive (PBX) materials with tensile properties being of particular interest. Direct tensile measurements using dogbone-shaped samples are considered the gold standard, but they are fairly large, making testing more costly and less desirable from a safety perspective. We investigated whether the measured tensile strength depends on the dogbone specimen size, which to our knowledge, has not been reported in the literature for PBX materials. Understanding this should inform the feasibility of employing smaller samples and how sample size should be considered when comparing PBX dogbone values in the literature. The TATB-based PBX dogbone sample size was varied by (a) scaling all dimensions proportionally and (b) varying only the length of the samples. It was observed that the measured tensile peak stress (strength) was a function of the sample size, and was more dependent on the diameter (cross-sectional area) than the length of the samples. Since peak stress is calculated as peak force normalized to the diameter of the sample, one might not expect an explicit diameter dependence for the peak stress. Therefore, these results suggest there may be an additional strengthening effect as the sample diameter is increased.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Particle trapping, size-filtering, and focusing in the nonthermal plasma synthesis of sub-10 nanometer particles

Low-pressure nonthermal flowing plasmas are widely used for the gas-phase synthesis of nanoparticles and quantum dots of materials that are difficult or impractical to synthesize using other techniques. To date, the impact of temporary electrostatic particle trapping in these plasmas has not been recognized, a process that may be leveraged to control particle properties. Furthermore, we present experimental and computational evidence that, during their growth in the plasma, sub-10 nm silicon particles become temporarily confined in an electrostatic trap in radio-frequency excited plasmas until they grow to a size at which the increasing drag force imparted by the flowing gas entrains the particles, carrying them out of the trap. We demonstrate that this trapping enables the size filtering of the synthesized particles, leading to highly monodisperse particle sizes, as well as the electrostatic focusing of the particles onto the reactor centerline. Understanding of the mechanisms and utilization of such particle trapping will enable the design of plasma processes with improved size control and the ability to grow heterostructured nanoparticles.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Probabilistic Sizing of Energy Storage Systems for Reliability and Frequency Security in Wind-Rich Power Grids

The penetration of wind energy has increased significantly in the power grid in recent times. Although wind is abundant, environment-friendly, and cheap, it is variable in nature and does not contribute to system inertia as much as conventional synchronous generators. Coupled with the low inertia contribution, the generation intermittency of wind power leads to reliability and stability issues in the power system. Energy storage systems (ESSs) are among the most prominent alternatives to alleviate these concerns associated with high wind penetration. This paper proposes a planning strategy to size ESS for the reliability and frequency security of wind-rich power grids. A probabilistic methodology for ESS sizing is developed utilizing a composite reliability-based framework with sequential Monte Carlo simulation (MCS). The MCS generates composite reliability indices for the power system, which are employed to obtain the capacity for a reliability energy storage system (RESS). Simultaneously, the MCS-derived probability of synchronization of conventional generators is integrated into an analytical approach for sizing a frequency support energy storage system (FESS). The effect of wind farm dispersion across geographical regions is incorporated in the framework to study possible reductions in the ESS size while maintaining the system reliability and frequency security. Furthermore, the efficacy of the proposed strategy is demonstrated on the RTS-GMLC test system.

25 ENERGY STORAGE↗
DOE OSTI2018

Application of the Model of Spheroidal Scatterers for Determination of Particles Sizes of Aqueous Suspensions by the Laser-Polarimetry and Dynamic-Light-Scattering Methods

Results of measurements of particle sizes of a dispersed medium by the methods of laser polarimetry and dynamic light scattering are presented for water suspensions of ZnO, CuO, TiO{sub 2}, and BaTiO{sub 3} with particles of irregular shape. When using the laser-polarimetry method, the particle-size distributions within the framework of the spheroidal-scatterer model are reconstructed. The same model was used to correct data obtained by the method of dynamic light scattering. The data obtained are compared with results obtained by electron microscopy. It is shown that, at values of the size parameter of 2–5, correction of the results of measurements obtained by the dynamic-light-scattering method makes it possible to reduce the error in determining the average particle size by this method to no more than 11%.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

The Effect of Temperature on the Particle Sizes and the Recrystallization of Silver Sulfide Nanopowders

The recrystallization of silver sulfide Ag{sub 2}S nanoparticles has been studied and the range of the thermal stability of the nanoparticle sizes has been determined. Nanopowders Ag{sub 2}S with particle sizes of 45–50 nm were obtained by chemical deposition from aqueous solutions. To study the thermal stability of the Ag{sub 2}S nanoparticle sizes, the nanocrystalline powders have been annealed in a vacuum of 0.01 Pa on heating from room temperature to 493 K and in argon at 623 K. Annealing up to a temperature of 453 K leads to insignificant nanoparticle growth and annealing of microstrains, which allows one to consider this temperature range as the region of thermal stability of the silver sulfide nanostate. The temperature range from 450 to 900 K, in which the particle size increases by a factor of 3–6, corresponds to the temperature of collective recrystallization of the silver sulfide nanopowder.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Model catalysis by size-selected cluster deposition

This report summarizes the accomplishments during the last four years of the subject grant. Results are presented for experiments in which size-selected model catalysts were studied under surface science and aqueous electrochemical conditions. Strong effects of cluster size were found, and by correlating the size effects with size-dependent physical properties of the samples measured by surface science methods, it was possible to deduce mechanistic insights, such as the factors that control the rate-limiting step in the reactions. Results are presented for CO oxidation, CO binding energetics and geometries, and electronic effects under surface science conditions, and for the electrochemical oxygen reduction reaction, ethanol oxidation reaction, and for oxidation of carbon by water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Comparison of particle sizes between 238 PuO 2 before aqueous processing, after aqueous processing, and after ball milling

Particle sizes determined for a single lot of incoming Russian fuel and for a lot of fuel after aqueous processing are compared with particle sizes measured on fuel after ball-milling. The single samples of each type are believed to have particle size distributions typical of oxide from similar lots, as the processing of fuel lots is fairly uniform. Variation between lots is, as yet, uncharacterized. Sampling and particle size measurement methods are discussed elsewhere.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗