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At least 847 records · Page 47

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DOE OSTI2017

Pd and Cu-Pd nanoparticles supported on multiwall carbon nanotubes for H{sub 2} detection

Highlights: • Pd and CuPd nanoparticles loaded on MWCNT have been used as H{sub 2}-sensors. • Promising H{sub 2} responses have been obtained in different atmospheres. • Electron transfer between nanoparticles and MWCNT is responsible for the detection. - Abstract: Simple, cost-effective, and reproducible devices have been prepared for the detection of H{sub 2} at room temperature. Pd, Cu and bimetallic Cu-Pd nanoparticles (prepared by the reduction-by-solvent method) have been loaded on a MWCNT deposit avoiding the use of surfactants or complicated techniques. The devices based on pure Pd nanoparticles have shown a high H{sub 2} sensitivity in the studied H{sub 2} concentration range with low response and recovery times. However, the addition of Cu in the metallic nanoparticles does not result in a considerable improvement. Furthermore, the Pd and Cu-Pd/MWCNTs-based sensors have kept part of their H{sub 2} sensitivity when they have been tested in an O{sub 2}-depleted atmospheres, which is an altogether new finding compared to Pd-based systems. Through these experiments it has been possible to conclude how the main H{sub 2} detection mechanism is the electron transfer from the nanoparticles (when the PdH{sub x} is formed) to the carbon nanotubes.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Aspect ratio control and photocatalytic properties analysis of anatase TiO2 nanoparticles

Highlights: • TiO{sub 2} nanoparticles with different aspect ratio were prepared and characterized. • Their aspect ratio is tuned by varying surfactants molar ratio and concentration. • TiO{sub 2} nanoparticles show photocatalytic activities in degradation of methylene blue. - Abstract: Anatase TiO{sub 2} nanoparticles with tuning size and aspect ratio were successfully prepared by a simple solvothermal method, using ethanol as a solvent, titanium butoxide as a precursor, and oleic acid and oleylamine as anionic and cationic capping agents, respectively. The average size and aspect ratio of these nanoparticles can be greatly regulated by varying the oleic acid/oleylamine molar ratio while keeping their total molar content constant and finely adjusted by increasing the total capping agents molar concentration in solvent at constant molar ratio (oleic acid/oleylamine molar ratio = 1:1). The variation of molar ratio or molar concentration enables a manipulation of the growth rate along different facets of TiO{sub 2} nanoparticles and, consequently, a control of the aspect ratio of these nanoparticles. Moreover, the photocatalytic degradation rate of methyl blue for sample prepared with molar ratio of oleic acid to oleylamine at 6:24 is over 11% higher than that for the other samples.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2021

New concept of radiolytic synthesis of gold nanoparticles in continuous flow

Radiolytic synthesis has been used to produce a plethora of unsupported and supported metallic nanoparticles in batch. As proof of a new concept, we evaluated the formation of gold nanoparticles by radiolytic synthesis in continuous flow using a millifluidic reactor. A mixture of gold ions solution, branched polyethyleneimine, and ethylene glycol yielded gold nanoparticles with a mean size of 3.4 ± 1.0 nm after irradiation with an X-ray irradiator (127 Gy/min) at an absorbed dose of 5.1 kGy. The morphology and size distribution of gold nanoparticles was influenced by AgNO 3 , where its absence resulted in a mean size of 20.9 ± 15.8 nm. The radiolytic synthesis of gold nanoparticles in continuous flow was achieved in short reaction times (<60 min), at room temperature, and with low concentrations of both stabilizing and reducing agents. Furthermore, these results demonstrate the potential of radiolytic synthesis in continuous flow for high-throughput formation of metallic nanoparticles with controlled specifications in size and distribution.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2014

Zinc oxide nanoparticles induce migration and adhesion of monocytes to endothelial cells and accelerate foam cell formation

Metal oxide nanoparticles are widely used in industry, cosmetics, and biomedicine. However, the effects of exposure to these nanoparticles on the cardiovascular system remain unknown. The present study investigated the effects of nanosized TiO{sub 2} and ZnO particles on the migration and adhesion of monocytes, which are essential processes in atherosclerogenesis, using an in vitro set-up of human umbilical vein endothelial cells (HUVECs) and human monocytic leukemia cells (THP-1). We also examined the effects of exposure to nanosized metal oxide particles on macrophage cholesterol uptake and foam cell formation. The 16-hour exposure to ZnO particles increased the level of monocyte chemotactic protein-1 (MCP-1) and induced the migration of THP-1 monocyte mediated by increased MCP-1. Exposure to ZnO particles also induced adhesion of THP-1 cells to HUVECs. Moreover, exposure to ZnO particles, but not TiO{sub 2} particles, upregulated the expression of membrane scavenger receptors of modified LDL and increased cholesterol uptake in THP-1 monocytes/macrophages. In the present study, we found that exposure to ZnO particles increased macrophage cholesterol uptake, which was mediated by an upregulation of membrane scavenger receptors of modified LDL. These results suggest that nanosized ZnO particles could potentially enhance atherosclerogenesis and accelerate foam cell formation. - Highlights: • Effects of metal oxide nanoparticles on foam cell formation were investigated. • Exposure to ZnO nanoparticles induced migration and adhesion of monocytes. • Exposure to ZnO nanoparticles increased macrophage cholesterol uptake. • Expression of membrane scavenger receptors of modified LDL was also increased. • These effects were not observed after exposure to TiO{sub 2} nanoparticles.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2023

Online detection of airborne nanoparticle composition with mass spectrometry: Recent advances, challenges, and opportunities

Airborne nanoparticles are receiving growing attention due to their impacts on human health, air quality, and climate. Additionally, there are increasing applications of aerosol-based nanotechnology. Real-time measurement of airborne nanoparticle composition is challenging due to their small masses and the difficulties in effectively separating them from larger particles. Custom-built instruments based on mass spectrometry have been developed for nanoparticle composition, including thermal desorption-based, laser-based, and solution-based techniques. They have significantly promoted the understanding of airborne nanoparticles in the last two decades. However, they are affected by molecular fragmentation, lack of mass-resolving power, incomplete species detection, and difficulties in directly comparing to gas-phase measurements. Recent developments in atmospheric mass spectrometry provide possible solutions. Here, this review presents the potential application of these new advances to real-time measurements of the molecular nanoparticle composition and discusses the associated challenges. Such measurements present opportunities for a more comprehensive view of airborne nanoparticles and their impacts.

47 OTHER INSTRUMENTATION↗

DOE OSTI2017

Fabrication of phosphonic acid films on nitinol nanoparticles by dynamic covalent assembly

Nitinol (NiTi) nanoparticles are a valuable metal alloy due to many unique properties that allow for medical applications. NiTi nanoparticles have the potential to form nanofluids, which can advance the thermal conductivity of fluids by controlling the surface functionalization through chemical attachment of organic acids to the surface to form self-assembled alkylphosphonate films. In this study, phosphonic functional head groups such as 16-phosphonohexadecanoic acid, octadecylphosphonic acid, and 12-aminododecylphosphonic acid were used to form an ordered and strongly chemically bounded film on the NiTi nanopowder. The surface of the NiTi nanoparticles was modified in order to tailor the chemical and physical properties to the desired application. The modified NiTi nanoparticles were characterized using infrared spectroscopy, powder X-ray diffraction, X-ray photoelectron spectroscopy, and 31 P solid-state nuclear magnetic resonance. The interfacial bonding was identified by spectroscopic data suggesting the phosphonic head group adsorbs in a mixed bidentate/monodentate binding motif on the NiTi nanoparticles. Dynamic light scattering and scanning electron microscopy-energy dispersive X-ray spectroscopy revealed the particle sizes. Differential scanning calorimetry was used to examine the phase transitions. Zeta potential determination as a function of pH was examined to investigate the surface properties of charged nanoparticles. In conclusion, the influence of environmental stability of the surface modifications was also assessed.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Protein nanoparticle vaccine based on flagellin carrier fused to influenza conserved epitopes confers full protection against influenza A virus challenge

Currently marketed influenza vaccines only confer protection against matching influenza virus strains. The influenza A composition of these vaccines needs to be annually updated. Vaccines that target conserved epitopes of influenza viruses would in principle offer broad cross-protection against influenza A viruses. In our study, we investigated the specific immune responses and protective efficacy of protein nanoparticles based on fusion proteins of flagellin carrier linked to conserved influenza epitopes. We designed fusion proteins by replacing the hyperimmunogenic region of flagellin (FliC) with four tandem copies of the ectodomain of matrix protein 2 (f4M2e), H1 HA2 domain (fHApr8) or H3 HA2 domain (fHAaichi). Protein nanoparticles fabricated from these fusion proteins by using DTSSP crosslinking retained Toll-like receptor 5 agonist activity of FliC. Intranasal immunization with f4M2e, f4M2e/fHApr8 or f4M2e/fHAaichi nanoparticles induced vaccine antigen-specific humoral immune responses. It was also found that the incorporation of the H1 HA2 domain into f4M2e/fHApr8 nanoparticles boosted M2e specific antibody responses. Immunized mice were fully protected against lethal doses of virus challenge. - Highlights: • Stable protein nanoparticles can be fabricated using DTSSP crosslinker. • Protein nanoparticles induce strong antibody responses against M2e and HA stalk domains in mice. • Vaccinated mice are fully protected against lethal dose of influenza A virus challenges.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2025

Precursor Identity and Surfactant Concentration Influence Shape of UO 2 Nanoparticles

A fundamental step toward studying the unique properties of actinide nanomaterials is control over the shape of actinide nanoparticles. Toward this goal, this work demonstrates the effects of precursor identity and surfactant concentration on the shape of uranium dioxide (UO 2 ) nanoparticles. UO 2 nanoparticles were synthesized by thermal decomposition of different precursors in the presence of oleylamine and oleic acid as surfactants. The size, shape, phase, and chemical composition of the nanoparticles was evaluated using transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS), electron diffraction (ED), and U L 3 -edge X-ray absorption fine-structure (XAFS) spectroscopy. Anisotropic UO 2 nanocubes of ∼ 4 nm were obtained only with low surfactant concentrations, while increasing the surfactant concentration resulted in formation of nanoparticles with an isotropic, sphere morphology. The importance of precursor identity was also investigated by employing U(hfa) 4 , U(acac) 4 , UO 2 (acac) 2 , and UO 2 (hfa) 2 ·H 2 O (where hfa = hexafluoracetylacetone and acac = acetylacetone) as precursors. The nanocube morphology was only observed when U(hfa) 4 was used as a precursor. XAS allowed for comparison of the disorder in anisotropic vs isotropic UO 2 nanoparticles.

Nanocubes↗

DOE OSTI2016

Enzymatically Controlled Vacancies in Nanoparticle Crystals

In atomic systems, the mixing of metals results in distinct phase behavior that depends on the identity and bonding characteristics of the atoms. In nanoscale systems, the use of oligonucleotides as programmable “bonds” that link nanoparticle “atoms” into superlattices allows for the decoupling of atom identity and bonding. While much research in atomic systems is dedicated to understanding different phase behavior of mixed metals, it is not well understood on the nanoscale how changes in the nanoscale “bond” affect the phase behavior of nanoparticle crystals. In this work, the identity of the atom is kept the same but the chemical nature of the bond is altered, which is not possible in atomic systems, through the use of DNA and RNA bonding elements. These building blocks assemble into single crystal nanoparticle superlattices with mixed DNA and RNA bonding elements throughout. The nanoparticle crystals can be dynamically changed through the selective and enzymatic hydrolysis of the RNA bonding elements, resulting in superlattices that retain their crystalline structure and habit, while incorporating up to 35% random vacancies generated from the nanoparticles removed. Therefore, the bonding elements of nanoparticle crystals can be enzymatically and selectively addressed without affecting the nature of the atom.

crystals↗

DOE OSTI2017

Diversifying Nanoparticle Assemblies in Supramolecule Nanocomposites Via Cylindrical Confinement

Many macroscopic properties such as collective chiral responses enhanced by coupled plasmonic nanoparticles require complex nanostructures. However, a key challenge is to directly assemble nanosized building blocks into functional entities with designed morphologies. For example, the DNA templated nanoparticle assembly has low scalability and requires aqueous conditions, while other approaches such as controlled drying and polymer templating access only simple 1-D, 2-D, and 3-D structures with limited assembly patterns. In this paper, we demonstrate a new self-assembly strategy that expands the diversity of 3-D nanoparticle assemblies. By subjecting supramolecular nanocomposites to cylindrical confinement, a range of new nanoparticle assemblies such as stacked rings and single and double helices can be readily obtained with a precisely defined morphology. Circular dichroism dark field scattering measurements on the single nanowire with Au helical ribbon-like assembly show chiral plasmonic response several orders of magnitude higher than that of natural chiral materials. The phase behavior of supramolecular nanocomposite under geometric constraints is quite different from that of block copolymer. Finally, it depends on the complex interplay among nanoparticle packing and phase behavior of parent block copolymers under confinement and can be governed by nanoparticle diffusion.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2018

Improving Quantum Yield of Upconverting Nanoparticles in Aqueous Media via Emission Sensitization

We demonstrate a facile method to improve upconversion quantum yields in Yb,Er-based nanoparticles via emission dye-sensitization. Using the commercially available dye ATTO 542, chosen for its high radiative rate and significant spectral overlap with the green emission of Er 3+ , we decorate the surfaces of sub-25 nm hexagonal-phase Na(Y/Gd/Lu) 0.8 F 4 :Yb 0.18 Er 0.02 upconverting nanoparticles with varying dye concentrations. Upconversion photoluminescence and absorption spectroscopy provide experimental confirmation of energy transfer to and emission from the dye molecules. Upconversion quantum yield is observed to increase with dye sensitization, with the highest enhancement measured for the smallest particles investigated (10.9 nm in diameter); specifically, these dye-decorated particles are more than 2× brighter than are unmodified, organic-soluble nanoparticles and more than 10× brighter than are water-soluble nanoparticles. We also observe 3× lifetime reductions with dye adsorption, confirming the quantum yield enhancement to result from the high radiative rate of the dye. As a result, the approach detailed in this work is widely implementable, renders the nanoparticles water-soluble, and most significantly improves sub-15 nm nanoparticles, making our method especially attractive for biological imaging applications.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Efficient Luminescence Enhancement of Mg{sub 2}TiO{sub 4}:Mn{sup 4+} Red Phosphor by Incorporating Plasmonic Ag@SiO{sub 2} Nanoparticles

One of prospective ways for boosting efficiency of luminescent materials is their combination with noble metal nanoparticles. Collective, so-called plasmon, oscillations of surface electrons in a nanoparticle can resonantly interact with incident or fluorescent light and cause an increase in the light absorption cross section or radiative rate for an adjacent emitter. Plasmonic inorganic phosphors require gentle host crystallization at which added noble nanoparticles will not suffer from aggregation or oxidation. The prospective plasmonic Mg{sub 2}TiO{sub 4}:Mn{sup 4+} phosphor containing core@shell Ag@SiO{sub 2} nanoparticles is prepared here by spare low-temperature annealing of a sol-gel host precursor. It is revealed that Mn{sup 4+} luminescence nonmonotonously depends on the size and concentration of 40 and 70 nm silver nanoparticles. It is demonstrated that luminescence of the Mg{sub 2}TiO{sub 4}:Mn{sup 4+} phosphor can be up to a 1.5 times increase when Mn{sup 4+} excitation is supported by localized surface plasmon resonance in Ag@SiO{sub 2} nanoparticles. © 2019 American Chemical Society.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2021

Discovery of Gold Nanoparticles in Marcellus Shale

A high density of gold (Au) nanoparticles has been observed on the surfaces of the coexisting opal nanospheres in kerogen-bearing shales from the Marcellus Formation. Our analyses of the Au nanoparticles and associated minerals indicate that this represents a new formation type of colloidal gold nanoparticles. Additionally, the opal nanospheres are a new kind of natural opal-A that is characteristic of the mesoporous texture formed through oil-in-water emulsion processes. High-resolution transmission electron microscopy (TEM) combined with energy-dispersive X-ray spectroscopy analysis directly reveals spherical gold nanoparticles and gold nanorods associated with mesoporous opal nanospheres. Our newly found textures indicate that opal nanospheres may have facilitated the co-precipitation of pure gold nanoparticles in organic-bearing, reduced environments. Furthermore, our TEM observations provide distinct images of the initial phase of colloidal gold and silica, which may contribute to the formation of Au deposits involving "invisible" gold, secondary supergene enrichments, or high-grade gold accumulations. Finally, the discovery of Au nanoparticles in hydrocarbon-rich shale formations such as Marcellus (which contains 0.6-4.1 wt % gold/opal) suggests a potential for co-production of both gas/oil and gold-two valuable commodities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Spatial Composition Influenced by Solvent in High-Entropy Alloy Nanoparticle Synthesis via Polyol Reduction

The performance of nanoparticles in catalytic reactions depends critically on their surface composition. In a multielemental system, this issue becomes even more important. Here, we report that the choice of solvent in polyol reduction synthesis of high entropy alloy (HEA) nanoparticles can have a subtle but significant influence on the elemental distribution near the surface of individual nanoparticles. Our study reveals that longchain polyethylene glycol typically produces a more uniform multielement distribution within a nanoparticle than short-chain triethylene glycol under identical experimental conditions. We performed electrochemical reduction of metal salts in both solvents to understand the reduction kinetics of metal salts, which shows that a solvent capable of improving the co-reduction of metal salts leads to the synthesis of more homogenized nanoparticles, whereas a solvent with a varying degree of reduction potency will lead to inhomogeneous elemental distribution in an HEA nanoparticle.

Catalyst↗

DOE OSTI2019

Sub-20 nm Core–Shell–Shell Nanoparticles for Bright Upconversion and Enhanced Förster Resonant Energy Transfer

Upconverting nanoparticles provide valuable benefits as optical probes for bioimaging and Förster resonant energy transfer (FRET) due to their high signal-to-noise ratio, photostability, and biocompatibility; yet, making nanoparticles small yields a significant decay in brightness due to increased surface quenching. Approaches to improve the brightness of UCNPs exist but often require increased nanoparticle size. Here we present a unique core-shell-shell nanoparticle architecture for small (sub-20 nm), bright upconversion with several key features: (1) maximal sensitizer concentration in the core for high near-infrared absorption, (2) efficient energy transfer between core and interior shell for strong emission, and (3) emitter localization near the nanoparticle surface for efficient FRET. This architecture consists of β-NaYbF 4 (core) @NaY 0.8-x Er x Gd 0.2 F 4 (interior shell) @NaY 0.8 Gd 0.2 F 4 (exterior shell), where sensitizer and emitter ions are partitioned into core and interior shell, respectively. Emitter concentration is varied (x = 1, 2, 5, 10, 20, 50, and 80%) to investigate influence on single particle brightness, upconversion quantum yield, decay lifetimes, and FRET coupling. We compare these seven samples with the field-standard core-shell architecture of β-NaY 0.58 Gd 0.2 Yb 0.2 Er 0.02 F 4 (core) @NaY 0.8 Gd 0.2 F 4 (shell), with sensitizer and emitter ions codoped in the core. At a single particle level, the core-shell-shell design was up to 2-fold brighter than the standard core-shell design. Further, by coupling a fluorescent dye to the surface of the two different architectures, we demonstrated up to 8-fold improved emission enhancement with the core-shell-shell compared to the core-shell design. Finally, we show how, given proper consideration for emitter concentration, we can design a unique nanoparticle architecture to yield comparable or improved brightness and FRET coupling within a small volume.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Electron beam induced evolution in Au, Ag, and interfaced heterogeneous Au/Ag nanoparticles

Sintering and sublimation process of nanoparticles made of Ag, Au, and interfaced Ag/Au heterodimers has been investigated by in-situ transmission electron microscopy at room temperature. Such process is driven by the illumination of high-energy electron beam accelerated at 200kV that promotes atom diffusion in the physically contacted nanoparticles. Upon electron illumination, adjacent Au nanoparticles gradually merge together to form a larger particle along with the reduction of surface area despite that orientated attachment is not observed. The nanoparticle fusion process is significantly different from the well-established thermal diffusion mechanism. In addition to the similar fusion process, Ag nanoparticles undergo apparent sublimation because the transferred energy from electron beam to nanoparticles is higher than the surface binding energy of Ag atoms when the electron scattering angle is larger than 112°. The electron beam illumination can transform the interfaced Au/Ag dimers to Au@Ag core-shell particles followed by a slow sublimation of the Ag shells. Both diffusion and sublimation of Ag atoms are dependent on the intensity of electron beam, i.e., higher beam intensity is favorable to accelerate both process.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Communication: Nanosize-induced restructuring of Sn nanoparticles

Stabilities and structures of β- and α-Sn nanoparticles are studied using density functional theory. Results show that β-Sn nanoparticles are more stable. For both phases of Sn, nanoparticles smaller than 1 nm (∼48 atoms) are amorphous and have a band gap between 0.4 and 0.7 eV. The formation of band gap is found to be due to amorphization. By increasing the size of Sn nanoparticles (1–2.4 nm), the degree of crystallization increases and the band gap decreases. In these cases, structures of the core of nanoparticles are bulk-like, but structures of surfaces on the faces undergo reconstruction. This study suggests a strong size dependence of electronic and atomic structures for Sn nanoparticle anodes in Li-ion batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Ultrashort laser ablation of bulk copper targets: Dynamics and size distribution of the generated nanoparticles

We address the role of laser pulse fluence on expansion dynamics and size distribution of the nanoparticles produced by irradiating a metallic target with an ultrashort laser pulse in a vacuum, an issue for which contrasting indications are present in the literature. To this end, we have carried out a combined theoretical and experimental analysis of laser ablation of a bulk copper target with ≈50 fs, 800 nm pulses, in an interval of laser fluencies going from few to several times the ablation threshold. On one side, molecular dynamics simulations, with two-temperature model, describe the decomposition of the material through the analysis of the evolution of thermodynamic trajectories in the material phase diagram, and allow estimating the size distribution of the generated nano-aggregates. On the other side, atomic force microscopy of less than one layer nanoparticles deposits on witness plates, and fast imaging of the nanoparticles broadband optical emission provide the corresponding experimental characterization. Both experimental and numerical findings agree on a size distribution characterized by a significant fraction (≈90%) of small nanoparticles, and a residual part (≈10%) spanning over a rather large size interval, evidencing a weak dependence of the nanoparticles sizes on the laser pulse fluence. Numerical and experimental findings show a good degree of consistency, thus suggesting that modeling can realistically support the search for experimental methods leading to an improved control over the generation of nanoparticles by ultrashort laser ablation.

77 NANOSCIENCE AND NANOTECHNOLOGY↗