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Breaking the Limit of Size-Dependent CO 2 RR Selectivity in Silver Nanoparticle Electrocatalysts through Electronic Metal–Carbon Interactions
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Plasmon-Driven Charge Transfer Aids Selective Nonthermal Vibrational Excitation in Nitrobenzenethiol on Silver Nanoparticles: Insights from Embedded Correlated Wavefunction Calculations
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Investigation of sex-based differences in the immunotoxicity of silver nanoparticles
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Electrically-generated memristor based on inkjet printed silver nanoparticles
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Printed Electrochemical Sensor for Quantifying Bone Density Loss in Microgravity
Printed electrochemical biosensors have been developed for astronaut point-of-care testing. Our fabrication approach is complimentary with in-space manufacturing for an on-demand and hands-free fabrication process. These sensors are developed using a combination of thin film materials printing and 3D printing and are comprised of carbon nanotube, gold nanoparticle, silver nanoparticle and dielectric inks to make traditional electrochemical sensor devices. Initial prototyped printed electrochemical sensors demonstrate good electrochemical performance while also displaying low batch to batch variability. Here we report the development of a printed sensor to monitor bone turnover. The absence of load bearing forces experienced in microgravity causes a reduction of overall bone mass and results in the development of space osteopenia/osteoporosis.(1,2) Our approach to identify space osteopenia/osteoporosis is to monitor the change in bone mass indirectly through an excreted biomarker of bone remodeling, amino-terminal collagen crosslinks (NTX). Antibodies specific to NTX are added to the sensor’s electrode ink and applied during the manufacturing process. NTX is measured from a urine sample by changes in voltammetry and electrochemical impedance as it binds to the antibody modified electrode surface. The measurement is rapid, quantitative and requires only small handheld electronics to perform the measurement. By this process, ground and flight physicians will receive frequent and real-time insight into the development of space osteopenia/osteoporosis to guide appropriate countermeasures. REFERENCES [1] Nabavi, N. et al (2011) Bone 49, 965-974. [2] Tamma, R. et al (2009) FASEB J 23, 2549-2554.
Engineering the Interface of Ceria and Silver Janus Nanoparticles for Enhanced Catalytic Performance in 4-Nitrophenol Conversion
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Aqueously Dispersed Silver Nanoparticle-Decorated Boron Nitride Nanosheets for Reusable, Thermal Oxidation-Resistant Surface Enhanced Raman Spectroscopy (SERS) Devices
The impurity-free aqueous dispersions of boron nitride nanosheets (BNNS) allowed the facile preparation of silver (Ag) nanoparticle-decorated BNNS by chemical reduction of an Ag salt with hydrazine in the presence of BNNS. The resultant Ag-BNNS nanohybrids remained dispersed in water, allowing convenient subsequent solution processing. By using substrate transfer techniques, Ag-BNNS nanohybrid thin film coatings on quartz substrates were prepared and evaluated as reusable surface enhanced Raman spectroscopy (SERS) sensors that were robust against repeated solvent washing. In addition, because of the unique thermal oxidation-resistant properties of the BNNS, the sensor devices may be readily recycled by short-duration high temperature air oxidation to remove residual analyte molecules in repeated runs. The limiting factor associated with the thermal oxidation recycling process was the Ostwald ripening effect of Ag nanostructures.
Translating nanoparticle dosimetry from conventional in vitro systems to occupational inhalation exposures
As encouraged by Toxicity Testing in the 21st Century, researchers increasingly apply high-throughput in vitro approaches to identify and characterize nanoparticle hazards, including conventional aqueous cell culture systems to assess respiratory hazards. Translating nanoparticle dose from conventional toxicity testing systems to relevant human exposures remains a major challenge for assessing occupational risk of nanoparticle exposures. Here, we explored existing computational tools and data available to translate nanoparticle dose metrics from cellular test systems to inhalation exposures of silver nanoparticles in humans. We used the Multiple-Path Particle Dosimetry (MPPD) Model to predict deposition of humans exposed to 20 and 110 nm silver nanoparticles at 0.9 µg/m3 over an 8 hr period, the proposed a National Institute of Occupational Safety and Health (NIOSH) recommended exposure limit (REL). MPPD predicts 1.88 and 0.98 µg of silver deposited in an 8 hr period for 20 and 110 nm nanoparticles, respectively, with 20 nm particles displaying nearly 11-fold higher total surface area deposited. Peak nanoparticle concentrations occurred more proximal in the pulmonary tract compared to mass deposition patterns (generation 5 vs. generations 20-21, respectively) due to regional differences in lung lining fluid volumes. Assuming 0.4% nanoparticle dissolution by mass as previously measured, we predict peak concentrations of silver ions in cells of 0.24 and 0.17 µg/mL for 20 and 110 nm particles, respectively. Both predicted concentrations are below the measured toxic threshold of 1.7 µg/mL of silver ions in cells from in vitro assessments. Assuming 4% dissolution by mass, we predict 10-fold higher silver concentrations in tissues, peaking at 2.4 and 1.7 µg/mL, for 20 and 110 nm nanoparticles respectively, exceeding the observed in vitro toxic threshold and highlighting the importance and sensitivity of dissolution rates. Overall, this approach offers a framework for extrapolating nanotoxicity results from in vitro cell culture systems to human exposures. Aligning appropriate dose metrics from in vitro and in vivo hazard characterizations and human pulmonary doses from occupational exposures are critical components for successful nanoparticle risk assessment and worker protection and provide guidance for designing future in vitro studies aimed at relevant human exposures.
Online ion mobility spectrometry of nanoparticle formation by non-thermal plasma conversion of metal salts in liquid aerosol droplets
The synthesis of nanoparticles by reaction of liquid aerosol droplets containing precursors in a flow-through, atmospheric-pressure, non-thermal plasma offers a continuous, scalable, substrate- and stabilizer-free approach for direct deposition into liquids or onto soft substrates. However, the combination of multiphase and non-equilibrium chemistry makes the process complicated and poorly understood. Here, we present ion mobility spectrometry measurements of liquid water droplets containing silver nitrate passing through an atmospheric-pressure dielectric barrier discharge reactor that allows us to monitor silver nanoparticle formation online for the first time. Mobility diameter distributions were obtained with the plasma on and off, and exhibited a shift, which was related to the degree of conversion of silver nitrate. The silver nanoparticles were also collected and characterized by UV–visible absorbance spectroscopy and transmission electron microscopy to support the online measurements. Importantly, negligible conversion was found when the water was removed by a diffusion dryer, suggesting that the key reducing species are in the liquid phase, such as solvated electrons. Finally, the study demonstrates how ion mobility spectrometry measurements can be applied to provide insight into this approach to nanoparticle synthesis.
Density Functional Tight Binding Insights into Plasmonic Silver–Platinum Nanoparticles and Alloys for Enhanced Photocatalysis
Developing accurate and efficient Slater-Koster (SK) tight-binding parameter sets is essential for quantum plasmonic studies of alloyed metal nanoparticles, as conventional time dependent density functional theory (TD-DFT) calculations are computationally prohibitive for larger clusters. In this work, we develop and validate density functional tight binding (DFTB) parameter sets for both ground state (GS-SK) and excited state (ES-SK) calculations to study the structural, electronic, and optical properties of silver (Ag), platinum (Pt), and Ag–Pt nanoalloys. Our investigation of the ground state properties demonstrates that the GS-SK parameters enable DFTB to closely reproduce the electronic structures of platinum clusters with diverse sizes and geometries – showing qualitative agreement with DFT for density of states (DOS) profiles and energy levels. The ES-SK parameters accurately describe excited-state properties compared to TD-DFT reference calculations, including the broad, featureless absorption profiles of Pt that are dominated by interband transitions. Using the ES-SK parameters within a real-time TD-DFTB framework, we compute size-dependent optical absorption spectra of Ag, Pt and Ag-Pt nanocubes containing up to 1099 atoms (size ∼4.18 nm). A detailed study of Ag–Pt and Pt-Ag core–shell nanoparticles shows quenching of the Ag plasmon resonance even at monolayer coverage for Ag-Pt, but not for Pt-Ag. We also show how to define submonolayer Ag-core Pt-shell cubic structures that have similar optical properties to those generated experimentally for much larger particles, which offers potential for describing plasmon-enhanced photocatalysis. Collectively, the GS-SK and ES-SK parameter sets provide an accurate, computationally efficient approach for modeling the complex optical and electronic behavior of noble–transition metal nanostructures and their alloys.
What happens to silver-based nanoparticles if they meet seawater?
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Stability and degradation mechanisms of silver–nickel nanoparticle catalysts for electrochemical CO 2 reduction
The Ni incorporation in the Ag–Ni alloy catalyst increases the density of active sites and promotes electron transfer between the active sites and reaction intermediates. A comparative investigation of the degradation mechanisms of pure Ag and Ag–Ni catalysts demonstrates that Ni incorporation suppresses surface reconstruction of the NPs, thereby enhancing the catalytic stability.
Capture of Iodine from Nuclear-Fuel-Reprocessing Off-Gas: Influence of Aging on a Reduced Silver Mordenite Adsorbent after Exposure to NO/NO 2
Iodine radioisotopes released during nuclear fuel reprocessing must be removed from the off-gas stream before discharge. One promising material for iodine capture is reduced silver mordenite (Ag 0 Z). Nevertheless, the adsorbent’s capacity will degrade, or age, over time when the material is exposed to other off-gas constituents. Though the overall impact of aging is known, the underlying physical and chemical processes are not. To examine these processes, Ag 0 Z samples were prepared and aged in 2% NO 2 in dry air and in 1% NO in N 2 gas streams at 150 °C for up to six months. Aged samples were then characterized using scanning electron microscopy, X-ray diffraction, Raman spectroscopy, and X-ray absorption spectroscopy. These techniques show that aging involves two overarching processes: (i) oxidation of the silver nanoparticles present in Ag 0 Z and (ii) migration of oxidized silver into the mordenite’s inner network. Silver on the nanoparticle’s surface is oxidized through adsorption of O 2 , NO, and NO 2 . Additionally, Raman spectroscopy and X-ray absorption spectroscopy indicate that nitrates are the primary products of this adsorption. Most of these nitrates migrate into the interior of the mordenite and exchange at framework binding sites, returning silver to its unreduced state (AgZ). The remaining nitrates exist at a persistent concentration without aggregating into bulk-phase AgNO 3 . X-ray absorption spectroscopy results further indicate that iodine adsorption occurs on not just Ag 0 Z but also on AgZ and a portion of the nitrates in the system. AgZ adsorbs a sizable quantity of iodine early in the aging process, but its capacity drops rapidly over time. For well-aged samples, nitrates are responsible for up to 95% of mordenite’s iodine capacity. Overall, these results have enhanced our understanding of the aging process in silver mordenite and are expected to guide the development of superior adsorbents for the capture of radioactive iodine from reprocessing off-gas.
Sulfides mediate the migration of nanoparticle mass out of nanocomposite plastics and into aqueous environments
We show that inorganic sulfides strongly influence transfer (migration) of nanoparticle mass out of polymer nanocomposites (PNCs) and into aqueous environments. We first manufactured two families of PNCs: one incorporating silver nanoparticles (AgNPs) and one incorporating CdSe quantum dots (QDs). Then, we assessed migration out of these PNCs and into aqueous media containing Na 2 S at concentrations ranging from 0 to 10 -4 M. Results show that Na 2 S strongly suppressed migration of Ag from AgNP-based PNCs: the migration into water spiked with 10 -6 M Na 2 S was 79% less than migration into water without Na 2 S, and no migration was detected (LOD ≈ 0.01 ng/cm 2 ) in water spiked with Na 2 S at 10 -5 M or 10 -4 M. With CdSe QD-based PNCs, Na 2 S suppressed Cd migration but enhanced Se migration, resulting in only a small net effect on the total QD migration but a large shift of the leachate composition (from favoring Cd by an average of 5.8 to 1 in pure water to favoring Se 9.4 to 1 when Na 2 S was present at 10 -4 M). These results show that common inorganic substances like sulfides may play a strong role in determining the environmental fate of polymer-dispersed nanoparticles and imply that migration tests conducted in purified water may not always accurately reflect migration into real environments.
Effect of grafting density on the two-dimensional assembly of nanoparticles
Employing grazing-incidence small-angle X-ray scattering (GISAXS) and X-ray reflectivity (XRR), we demonstrate that films composed of polyethylene glycol (PEG)-grafted silver nanoparticles (AgNPs) and gold nanoparticles (AuNPs), as well as their binary mixtures, form highly stable hexagonal structures at the vapor–liquid interface. These nanoparticles exhibit remarkable stability under varying environmental conditions, including changes in pH, mixing concentration, and PEG chain length. Short-chain PEG grafting produces dense, well-ordered films, while longer chains produce more complex, less dense quasi-bilayer structures. AuNPs exhibit higher grafting densities than AgNPs, leading to more ordered in-plane arrangements. In binary mixtures, AuNPs dominate the population at the surface, while AgNPs integrate into the system, expanding the lattice without forming a distinct binary superstructure. In conclusion, these results offer valuable insights into the structural behavior of PEG-grafted nanoparticles and provide a foundation for optimizing binary nanoparticle assemblies for advanced nanotechnology applications.
Titanium dioxide and table sugar enhance the leaching of silver out of nanosilver packaging
We manufactured laboratory-scale food packages containing 2.57 ± 0.18 × 10 –3 wt% silver nanoparticles (AgNPs) and used them to show that table sugar (sucrose) and microcrystalline titanium dioxide (μTiO 2 ) enhance Ag migration from these packages and into aqueous food simulants. Ag migration into purified water was detected but was below the limit of ICP-MS quantitation, giving a range of potential Ag migration between 0.059 and 0.082 ng cm –2 packaging surface area. Ag migration into 9 wt% aqueous sucrose solution was 0.547 ± 0.084 ng cm –2 and migration into 9 wt% sucrose solution containing 0.01 wt% μTiO 2 was 0.724 ± 0.032 ng cm –2 . Total Ag migration into a 0.01 wt% μTiO 2 aqueous dispersion without sucrose was between 0.122 and 0.162 ng cm –2 , with upper and lower limits defined by the detectability of Ag in the supernatant phase of the simulant. If the midpoint of this range is taken as a baseline, these results imply that, compared to purified water, Ag migration was increased by approximately 10.3 times when the water simulant contained μTiO 2 and sucrose at commercially-relevant concentrations. Notably, the Ag migrated into water containing both ingredients exceeded the total Ag migrated into either of the single-ingredient simulants, pointing to a potential cooperative relationship between sucrose and μTiO 2 that possibly derives from binding and redox interactions between these two ingredients. Sucrose and μTiO 2 also both reduced a portion of migrated Ag + back into AgNPs, and μTiO 2 particles efficiently captured (>25% by mass) migrated Ag on their surfaces. Similar effects on migration were observed with nanocrystalline TiO 2 . Furthermore, these experiments are the first to show that TiO 2 particles exert a strong influence on the quantity and form of Ag that could migrate from AgNP-enabled packaging, suggesting that food formulations and interactions between individual food components may be important to consider when evaluating the fate of nanoparticles in these consumer applications.