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SUMMARY REPORT FOR ZINC 65 CONTAMINATION CONTROL

Radioactive zinc, {sup 65}Zn, was detected after extraction of 215 TPBARs in from TVA reactor fuel cycle 6. A team consisting of Tritium Engineering, Tritium Operations, Tritium Radiation Control, and Savannah River National Laboratory personnel evaluated the risk and response and developed short, medium and long term goals for contamination control. One of the goals was incorporated into site Performance Based Incentive CO 3.4, to optimize the filter geometry and operating conditions for the Tritium Extraction Facility. This goal included a scoping study to determine if the contamination could be contained within the high radiation environment of the furnace module as well. In order to optimize the filters studies were conducted to independently evaluate the effect of pore size on pumping efficiency and zinc trapping efficiency (1). A study was also conducted to evaluate the effect of temperature on the trapping efficiency and adhesion (2). In addition, the potential for chemically trapping zinc in the lithium trap was evaluated using a thermodynamic study (3) followed by preliminary experimental testing (4). Based on the work that was completed it is determined that a 20 {mu}m filter heated to between 120 and 200 C will act as an effective physical trap for zinc vapors. It may be possible to chemically react zinc with copper or cobalt to form zinc intermetallic compounds or alloys but additional work under more prototypic conditions are required.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analysis of Zinc 65 Contamination after Vacuum Thermal Process

Radioactive contamination with a gamma energy emission consistent with {sup 65}Zn was detected in a glovebox following a vacuum thermal process. The contaminated components were removed from the glovebox and subjected to examination. Selected analytical techniques were used to determine the nature of the precursor material, i.e., oxide or metallic, the relative transferability of the deposit and its nature. The deposit was determined to be borne from natural zinc and was further determined to be deposited as a metallic material from vapor.

 Contamination↗

Bronze Alloy Development for Zinc Vapor Capture

After gamma-emitting 65 Zinc was detected in a vacuum pumping system contained in a tritium glovebox, a series of experiments were undertaken to develop a method and material to trap zinc vapors in an area that is more suitable for preventing dose to workers. In this study, bronze alloys with 0–30% tin were prepared using a powder metallurgical process and exposed to three levels of zinc vapors. Furthermore, all of the alloys demonstrated acceptable zinc gettering capacity; however, low tin content bronzes are considered for further testing.

36 MATERIALS SCIENCE↗

Methods of Preventing the Spread of Zinc Contamination During Vacuum Processing

Radioactive zinc, 65 Zn, was detected after a thermal vacuum process that extracted a desired product from articles out of a commercial light water reactor. While the facility is designed to handle radioactive materials, the location of the 65 Zn was in an area that is not designed for gamma emitting contaminants. A series of experiments were conducted to entrain the contaminant in an easily replaceable trap within the process piping. The experiments were conducted with increasing levels of complexity. Initially a simple apparatus was developed to determine the effect of substrate temperature on the vapor capture, this was followed by experiments to determine the effect of filter pore size on pumping and trapping, finally the interactive effects of both pore size and temperature were evaluated. The testing was conducted on a system that used a roughing vacuum pump using model and prototypic materials. It was determined that heating the substrate to nominally 200°C resulted in effective trapping on the model as well as prototypic material.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Nuclear Data Sheets for A = 65

The evaluators present in this publication spectroscopic data and level schemes from radioactive decay and nuclear reactions studies for all isobars with mass number A=65. Not much is known experimentally about {sup 65}V and {sup 65}Cr, although they are expected to decay by {beta}-emission. Spin/parity assignments for {sup 65}Mn, {sup 65}Fe, {sup 65}As, and {sup 65}Se are not firmly established.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fast-Neutron Activation of Long-Lived Isotopes in Enriched Ge

We measured the production of 57Co, 54Mn, 68Ge, 65Zn, and 60Co in an sample of Ge enriched in isotope 76 due to high-energy neutron interactions. These isotopes are critical in understanding background in Ge detectors used for double-beta decay experiments. These isotopes are produced by cosmogenic-neutron interactions in the detectors while they reside on the Earth's surface. We compared the measured production to that predicted by cross-section calculations based on CEM03.02. The cross section calculations over-predict our measurements by approximately a factor of 2-3 depending on isotope. We then use the measured cosmic-ray neutron ux and our results to predict the cosmogenic production rate with an accuracy near 15%.

Environmental Molecular Sciences Laboratory↗

β Decay in the Region of Neutron-deficient {sup 69,70,71}Kr

Decay spectroscopy was performed for neutron-deficient nuclei ranging from zinc to krypton with isospin −3/2 ≤T{sub z}≤0. Measurements of correlated β-delayed protons allowed us to determine the isobaric analog states fed from the decay of {sup 65}Se and {sup 69}Kr, constraining the spin of the {sup 69}Kr ground state. Preliminary results regarding the half lives for the T{sub z}=−1 systems, relevant to the rapid proton capture (rp) process, are discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Search for sterile neutrinos in gallium experiments with artificial neutrino sources

The possibility of the BEST experiment on electron neutrino disappearance with intense artificial sources of electron neutrino {sup 51}Cr is considered. BEST has the great potential to search for transitions of active neutrinos to sterile states with Δm{sup 2} ∼ 1 eV{sup 2} and to set the limits on short baseline electron neutrino disappearance oscillation parameters. The possibility of the further constraints the oscillation parameters region with using {sup 65}Zn source is discussed.

07 ISOTOPE AND RADIATION SOURCES↗

Intercalation of Nanopolyaniline with Nanobentonite and Manganese Oxide Nanoparticles as a Novel Nanocomposite to Remediate Cobalt/Zinc and Their Radioactive Nuclides {sup 60}Co/{sup 65}Zn

A novel nanocomposite based on the combination of nanobentonite with nanopolyaniline and nanomanganese oxide (N-Bent–NPANI–NMn{sub 3}O{sub 4}) was synthesized and investigated to extract Co/Zn ions from water using batch technique and {sup 60}Co/{sup 65}Zn radionuclides from radioactive wastewater using column techniques. Characterization was established by High resolution-transmission electron microscopy (HR-TEM), Scanning electron microscope, X-ray diffraction (XRD), thermal gravimetric analysis (TGA) and Fourier transform infrared spectrophotometer. The image of HR-TEM indicated that the produced nanocomposite was ranged from 59.07 to 83.38 nm. Solution pH, time of reaction, amount of solid and metal concentration, all of these parameters were inspected and optimized as fundamental factors during the extraction process. The obtained results implied that the ideal conditions for extraction were pH 6 and 7, reaction time 10 and 20 min, for Co and Zn ions, respectively. The highest removal capacities were found 255.28 and 202.22 mg g{sup −1} for Co and Zn, respectively by using 5 mg nanocomposite. Excellent recoveries were obtained as 94.0–94.5% and 92.0–93.0% for removal of Co–{sup 60}Co and of Zn–{sup 65}Zn ions, respectively from the examined samples. Graphical Abstract: .

77 NANOSCIENCE AND NANOTECHNOLOGY↗

The characteristic assessment of spent ion exchange resin from PUSPATI TRIGA REACTOR (RTP) for immobilization process

In this paper, spent ion exchange resin generated from PUSPATI TRIGA reactor (RTP) in Malaysian Nuclear Agency were characterized based on the water content, radionuclide content and radionuclide leachability. The result revealed that the water content in the spent resin is 48%. Gamma spectrometry analysis indicated the presence of {sup 134}Cs, {sup 137}Cs, {sup 152}Eu, {sup 54}Mn, {sup 58}Co, {sup 60}Co and {sup 65}Zn. The leachability test shows a small concentrations (<1 Bq/l) of {sup 152}Eu and {sup 134}Cs were leached out from the spent resin while {sup 60}Co activity concentrations slightly exceeded the limit generally used for industrial wastewater i.e. 1 Bq/l. Characterization of spent ion exchange resin sampled from RTP show that this characterization is important as a basis to immobilize this radioactive waste using geopolymer technology.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

MoS{sub 2}@ZnO nano-heterojunctions with enhanced photocatalysis and field emission properties

The molybdenum disulfide (MoS{sub 2})@ZnO nano-heterojunctions were successfully fabricated through a facile three-step synthetic process: prefabrication of the ZnO nanoparticles, the synthesis of MoS{sub 2} nanoflowers, and the fabrication of MoS{sub 2}@ZnO heterojunctions, in which ZnO nanoparticles were uniformly self-assembled on the MoS{sub 2} nanoflowers by utilizing polyethyleneimine as a binding agent. The photocatalytic activities of the composite samples were evaluated by monitoring the photodegradation of methylene blue (MB). Compared with pure MoS{sub 2} nanoflowers, the composites show higher adsorption capability in dark and better photocatalytic efficiency due to the increased specific surface area and improved electron-hole pair separation. After irradiation for 100 min, the remaining MB in solution is about 7.3%. Moreover, the MoS{sub 2}@ZnO heterojunctions possess enhanced field emission properties with lower turn-on field of 3.08 V μm{sup −1}and lower threshold field of 6.9 V μm{sup −1} relative to pure MoS{sub 2} with turn-on field of 3.65 V μm{sup −1} and threshold field of 9.03 V μm{sup −1}.

36 MATERIALS SCIENCE↗

Phonon thermodynamics and elastic behavior of GaN at high temperatures and pressures

The effects of temperature and pressure on the phonons of GaN were calculated for both the wurtzite and zinc-blende structures. In this work, the quasiharmonic approximation (QHA) gave reasonable results for the temperature dependence of the phonon DOS at zero pressure but unreliably predicted the combined effects of temperature and pressure. Pressure was found to change the explicit anharmonicity, altering the thermal shifts of phonons and more notably qualitatively changing the evolution of phonon lifetimes with increasing temperature. These effects were largest for the optical modes, and phonon frequencies below approximately 5 THz were adequately predicted with the QHA. The elastic anisotropies of GaN in both wurtzite and zinc-blende structures were calculated from the elastic constants as a function of pressure at 0 K. The elastic anisotropy increased with pressure until reaching elastic instabilities at 40 GPa (zinc blende) and 65 GPa (wurtzite). The calculated instabilities are consistent with proposed transformation pathways to rocksalt GaN and place upper bounds on the pressures at which wurtzite and zinc-blende GaN can be metastable.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

PRELIMINARY STUDY OF METHODS TO CHEMICALLY BIND ZINC

To address the {sup 65}Zn contamination issue in the TEF, a multi-task experimental program was initiated. The first two experimental tasks were completed. The results of the third experimental task are reported here. This task was conducted to determine if the zinc vapors could be chemically bound on two non hydrogen active substrates. Based on a thermodynamic study copper and cobalt were the most favorable for capturing zinc without forming hydrides. Within the experimental parameters tested, which include temperatures of 350, 400, and 450 C at pressures of nominally 20-40 millitorr, the zinc deposited on the both copper screen and cobalt rods but did not react to form a compound. The conditions that were tested are not prototypic and additional testing under higher vacuum conditions, i.e., .01 millitorr, may enhance the reactivity of the surfaces and is recommended.

08 HYDROGEN↗

Wide-angle antireflection ZnO films on bullet-like nanostructures of multi-crystalline silicon

Nanosphere lithography and antireflection coating techniques have been applied to fabricate wide-angle antireflection structures on multicrystalline silicon substrates. Self-assembled 550-nm SiO{sub 2} nanospheres were arranged periodically to act as a mask to block the inductively coupled plasma dry etching and form bulletlike nanostructures on the surface of the multicrystalline silicon wafer. Then a 65-nm-thick zinc oxide film was deposited on the nanostructures using the atomic layer deposition method. The results show that when applying the nanostructure with a ZnO film the average reflectivity of the multicrystalline silicon wafer can be decreased from 36% to 0.65% in the wavelength range from 400 nm to 850 nm for an incident angle of 8 deg. . When the incident angle reaches 60 deg. the average reflectivity of the sample becomes less than 4.6%.

36 MATERIALS SCIENCE↗

EFFECT OF FILTER TEMPERATURE ON TRAPPING ZINC VAPOR

To address the {sup 65}Zn contamination issue in the TEF, a multi-task experimental program was initiated. The first experimental task was completed and is reported in Ref. 1. The results of the second experimental task are reported here. This task examined the effect of filter temperature on trapping efficiency and deposit morphology. Based on the first experimental tasks that examined filter pore size and trapping efficiency, stainless steel filter media with a 20 {micro}m pore size was selected. A series of experiments using these filters was conducted during this second task to determine the effect of filter temperature on zinc vapor trapping efficiency, adhesion and morphology. The tests were conducted with the filters heated to 60, 120, and 200 C; the zinc source material was heated to 400 C for all the experiments to provide a consistent zinc source. The samples were evaluated for mass change, deposit adhesion and morphology. As expected from the physical vapor deposition literature, a difference in deposit morphology and appearance was observed between the three filter temperatures. The filter held at 60 C had the largest average mass gain while the 120 and 200 C filters exhibited similar but lower weight gains. The standard deviations were large and suggest that all three temperatures exhibited comparable gains. No zinc was detected on the backside surface of the filters indicating high efficiency for front and internal trapping. A zinc rich deposit was formed on the surface of the 60 C filter. Based on a simple tape adhesion test, the surface zinc was readily removed from the 60 C filter while less zinc deposit was removed from the 120 and 200 C filter samples. It is surmised that the higher temperatures enable the zinc to deposit within the filter media rather than on the surface. Based on the findings that all three statistically trapped the same quantity of zinc vapor and that the higher temperatures resulted in a more adherent/better trapped product, operating the filters at 120 to 200 C is recommended.

36 MATERIALS SCIENCE↗

Nuclear import of cutaneous beta genus HPV8 E7 oncoprotein is mediated by hydrophobic interactions between its zinc-binding domain and FG nucleoporins

We have previously discovered and characterized the nuclear import pathways for the E7 oncoproteins of mucosal alpha genus HPVs, type 16 and 11. Here we investigated the nuclear import of cutaneous beta genus HPV8 E7 protein using confocal microscopy after transfections of HeLa cells with EGFP-8E7 and mutant plasmids and nuclear import assays in digitonin-permeabilized HeLa cells. We determined that HPV8 E7 contains a nuclear localization signal (NLS) within its zinc-binding domain that mediates its nuclear import. Furthermore, we discovered that a mostly hydrophobic patch {sub 65}LRLFV{sub 69} within the zinc-binding domain is essential for the nuclear import and localization of HPV8 E7 via hydrophobic interactions with the FG nucleoporins Nup62 and Nup153. Substitution of the hydrophobic residues within the {sub 65}LRLFV{sub 69} patch to alanines, and not R66A mutation, disrupt the interactions between the 8E7 zinc-binding domain and Nup62 and Nup153 and consequently inhibit nuclear import of HPV8 E7. - Highlights: • HPV8 E7 has a cNLS within its zinc-binding domain that mediates its nuclear import. • Discovery of a hydrophobic patch that is critical for the nuclear import of HPV8 E7. • HPV8 E7 nuclear import is mediated by hydrophobic interactions with FG-Nups, Nup62 and Nup153.

60 APPLIED LIFE SCIENCES↗

Copper doping of ZnO crystals by transmutation of {sup 64}Zn to {sup 65}Cu: An electron paramagnetic resonance and gamma spectroscopy study

Transmutation of {sup 64}Zn to {sup 65}Cu has been observed in a ZnO crystal irradiated with neutrons. The crystal was characterized with electron paramagnetic resonance (EPR) before and after the irradiation and with gamma spectroscopy after the irradiation. Major features in the gamma spectrum of the neutron-irradiated crystal included the primary 1115.5 keV gamma ray from the {sup 65}Zn decay and the positron annihilation peak at 511 keV. Their presence confirmed the successful transmutation of {sup 64}Zn nuclei to {sup 65}Cu. Additional direct evidence for transmutation was obtained from the EPR of Cu{sup 2+} ions (where {sup 63}Cu and {sup 65}Cu hyperfine lines are easily resolved). A spectrum from isolated Cu{sup 2+} (3d{sup 9}) ions acquired after the neutron irradiation showed only hyperfine lines from {sup 65}Cu nuclei. The absence of {sup 63}Cu lines in this Cu{sup 2+} spectrum left no doubt that the observed {sup 65}Cu signals were due to transmuted {sup 65}Cu nuclei created as a result of the neutron irradiation. Small concentrations of copper, in the form of Cu{sup +}-H complexes, were inadvertently present in our as-grown ZnO crystal. These Cu{sup +}-H complexes are not affected by the neutron irradiation, but they dissociate when a crystal is heated to 900 °C. This behavior allowed EPR to distinguish between the copper initially in the crystal and the copper subsequently produced by the neutron irradiation. In addition to transmutation, a second major effect of the neutron irradiation was the formation of zinc and oxygen vacancies by displacement. These vacancies were observed with EPR.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗