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At least 73 records · Page 4

The Use of Silver Chloride Injection in Remediation of Iodine-129 by In Situ Capture as Silver Iodide at the F-Area Seepage Basin - 20225

The Savannah River Site (SRS) produced tritium, plutonium, and special nuclear materials for national defense, medicine, and the space programs. As part of operations, the F-Area Seepage Basins operated until 1988 for the disposition of deionized acidic wastewater from the F Separations Facility. The wastewater contained dilute nitric acid and low concentrations of non-radioactive metals, and radionuclides, with the major isotopes being Cs-137, Sr-90, U-235, U-238, Pu-239, Tc-99, I-129, and tritium. The seepage basins were closed in 1988 and backfilled and capped by 1991. The groundwater emanating from beneath the closed and capped seepage basins is acidic and contains elevated levels of both chemical and radiological contaminants. Releases from the groundwater plumes sourced from the F-Area Seepage Basins have impacted the water quality of Fourmile Branch, which is a small tributary to the Savannah River, a regional water source. A large pump-and-treat system was constructed in 1997 and operated until 2003 in an attempt to capture the releases to Fourmile Branch. The system in F Area and a similar system in H Area were expensive (∼$1.3 M/month) to operate and produced large quantities of radioactive waste, with concentrations of I- 129 too high to be disposed of at the SRS. In 2004, SRS replaced pump-and-treat with a funnel and gate system that along with operation of a base injection system at the gates reduces the flux of contaminants to the wetlands adjacent to Fourmile Branch. The alkaline solution injected into the aquifer neutralizes the acidic plume and immobilizes many of the cationic constituents. However, base injection is not effective in managing the release of iodine-129, an anionic contaminant. To address iodine-129 SRS and the Savannah River National Laboratory developed an in situ technology that uses ultra-fine ground silver chloride (AgCl) as an injectable capture medium for the sequestration of iodine-129. The AgCl amendment has a very small particle size and is designed to be injected into the contaminated aquifer to capture iodine-129. Dissolved iodine-129 forms a stable and highly insoluble solid (silver iodide) upon contact with AgCl. Laboratory studies, a field scale pilot test (2009), and three deployments (2011, 2015 and 2019) of AgCl have been successfully performed at the F-Area Seepage Basins. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Structural Defects of Silver Hollandite, Ag x Mn 8 O y , Nanorods: Dramatic Impact on Electrochemistry

Hollandites (OMS-2) are an enticing class of sorbents, catalysts, and energy storage materials with a tunnel structure permitting one-dimensional insertion and deinsertion of ions and small molecules along the c direction. A 7-fold increase in delivered capacity for Li/Ag x Mn 8 O 16 electrochemical cells (160 versus 23 mAh/g) observed upon a seemingly small change in silver content ( x ~1.1 (L-Ag-OMS-2) and 1.6 (H-Ag-OMS-2)) led us to characterize the structure and defects of the silver hollandite material. In this work, Ag hollandite nanorods are studied through the combined use of local (atomic imaging, electron diffraction, electron energy-loss spectroscopy) and bulk (synchrotron based X-ray diffraction, thermogravimetric analysis) techniques. Selected area diffraction and high resolution transmission electron microscopy show a structure consistent with that refined by XRD; however, the Ag occupancy varies significantly even within neighboring channels. Both local and bulk measurements indicate a greater quantity of oxygen vacancies in L-Ag-OMS-2, resulting in lower average Mn valence relative to H-Ag-OMS-2. Electron energy loss spectroscopy shows a lower Mn oxidation state on the surface relative to the interior of the nanorods, where the average Mn valence is approximately Mn 3.7+ for H-Ag-OMS-2 and Mn 3.5+ for L-Ag-OMS-2 nanorods, respectively. The higher delivered capacity of L-Ag-OMS-2 may be related to more oxygen vacancies compared to H-Ag-OMS-2. Thus, the oxygen vacancies and MnO 6 octahedra distortion are assumed to open the MnO 6 octahedra walls, facilitating Li diffusion in the ab plane. These results indicate crystallite size and surface defects are significant factors affecting battery performance.

25 ENERGY STORAGE↗

K{sub α} and bremsstrahlung x-ray radiation backlighter sources from short pulse laser driven silver targets as a function of laser pre-pulse energy

Measurements of silver K-shell and bremsstrahlung emission from thin-foil laser targets as a function of laser prepulse energy are presented. The silver targets were chosen as a potential 22 keV backlighter source for the National Ignition Facility Experiments. The targets were irradiated by the Titan laser with an intensity of 8 × 10{sup 17} W/cm{sup 2} with 40 ps pulse length. A secondary nanosecond timescale laser pulse with controlled, variable energy was used to emulate the laser prepulse. Results show a decrease in both K{sub α} and bremsstrahlung yield with increasing artificial prepulse. Radiation hydrodynamic modeling of the prepulse interaction determined that the preplasma and intact target fraction were different in the three prepulse energies investigated. Interaction of the short pulse laser with the resulting preplasma and target was then modeled using a particle-in-cell code PSC which explained the experimental results. The relevance of this work to future Advanced Radiographic Capability laser x-ray backlighter sources is discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Effect of multipole excitations in electron energy-loss spectroscopy of surface plasmon modes in silver nanowires

We have characterized the surface plasmon resonance (SPR) in silver nanowires using spatially resolved electron energy loss spectroscopy (EELS) in the scanning transmission electron microscope. Non-symmetric EELS spectra due to high-k SPR propagation along the nanowire and spectral shifts due to higher-order mode excitation are observed when the beam is positioned near the tip of the nanowire. When the beam is far from the tip region and on the side of nanowire, no spectral shifts are observed as the beam is scanned in the radial direction of the nanowire. The experimental spectra are compared with three different theoretical approaches: direct numerical calculation of the energy loss, analytical models for energy loss, and numerical simulations using an optical model. All three models reproduce the spectral shifts as the electron beam approaches the cap of the nanowire. The analytical model reveals the origin of the shifts in high-order plasmon mode excitation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Optical properties and plasmonic response of silver-gallium nanostructures

Silver and gallium form an alloy Ag{sub 2}Ga via a room temperature spontaneous self-assembly that exhibits remarkable mechanical and electrical properties suitable for nanoscale measurements. However, whether photon excitation of plasmons in this emerging nanomaterial is retained or not has not been established. Here, we present a thin film formation of Ag{sub 2}Ga via a spreading-reactive process of liquid Ga on an Ag film and a characterization of its dielectric function ϵ(E) = ϵ{sub 1}(E) + iϵ{sub 2}(E) in the photon energy range 1.42 eV ≤ E < 4.2 eV. It is observed that while the plasmon damping increases, near an energy of 2.25 eV, the real part of ϵ exhibits a crossing with respect to that of Ag. Furthermore, the impact of new plasmon supporting materials is discussed and in order to enable further applications in plasmonics, the possibility of photon excitation of surface plasmons in Ag{sub 2}Ga is studied.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Influence of annealing on the photodeposition of silver on periodically poled lithium niobate

The preferential deposition of metal nanoparticles onto periodically poled lithium niobate surfaces, whereby photogenerated electrons accumulate in accordance with local electric fields and reduce metal ions from solution, is known to depend on the intensity and wavelength of the illumination and the concentration of the solution used. Here, it is shown that for identical deposition conditions (wavelength, intensity, concentration), post-poling annealing for 10 h at 200 °C modifies the surface reactivity through the reorientation of internal defect fields. Whereas silver nanoparticles deposit preferentially on the +z domains on unannealed crystals, the deposition occurs preferentially along 180° domain walls for annealed crystals. In neither case is the deposition selective; limited deposition occurs also on the unannealed –z domain surface and on both annealed domain surfaces. The observed behavior is attributed to a relaxation of the poling-induced defect frustration mediated by Li{sup +} ion mobility during annealing, which affects the accumulation of electrons, thereby changing the surface reactivity. The evolution of the defect field with temperature is corroborated using Raman spectroscopy.

36 MATERIALS SCIENCE↗