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Isotopically anomalous xenon in meteorites - A new clue to its origin

The CCF xenon component in primitive meteorites, which has been attributed either to fission of a superheavy element or to nucleosynthesis in a supernova, does not show the large enrichment in Xe-129 (from decay of 16 Myr I-129) expected for supernova ejecta. Although this problem can be circumvented by ad hoc assumptions, a fission origin of CCFXe seems more likely.

Lewis, R. S.↗

Xenon and other noble gases in shergottites

The isotopic composition of the xenon component trapped in EETA 79001's lithologies B and C has been determined, and other noble gases were measured in some samples. The Xe component was found to have light isotope ratios indistinguishable from those of the terrestrial atmosphere. The trapped component has a Xe-129/Xe-132 ratio of about 2.4, and is enhanced in Xe-134 and Xe-136 relative to the terrestrial atmosphere or the average carbonaceous chondrite. Similarities between values for Ar-40/Ar-36, Xe-129/Xe-132, and N-15/N-14 and the corresponding Martian atmospheric values suggest Martian origin of the trapped gases.

Swindle, T. D.↗

Noble gases in the howardites Bholghati and Kapoeta

Analyses of noble gases in whole rock samples of the howardites Bholghati and Kapoeta and grain-size separates of Kapoeta yield evidence for excesses of the Xe isotopes Xe-129 , Xe-131, Xe-132, Xe-134, and Xe-136 in a low-temperture component, similar to lunar excess fission Xe. Such a component may be able to provide chronometric information if the relative abundances of radioactive progenitors (I-129, Pu-244, and U-238) can be determined, but the isotopic spectra obtained are not sufficiently precise to do so. Eucritic clast BH-5 in Bholghati contains Xe produced in situ by the decay of Pu-244. Calculated fission Xe retention ages are 30-70 Ma after the formation of the solar system, consistent with the apparent presence of Sm-146 decay products. Both the clast and the matrix of Bholghati have K-Ar ages of about 2 Ga, suggesting a common thermal event at least that recently.

Swindle, T. D.↗

Comparative xenology of two angrites

Results are presented on Xe analysis during stepwise heating of the angrite meteorite Lewis Cliff 86010 and the Angra dos Reis angrite. It is shown that both the Lewis Cliff and the Angra dos Reis angrites are poor in trapped Xe and are rich in fission Xe from Pu-244 and in spallation Xe produced by cosmic ray irradiation of Ba and the light REE, and that neither meteorite has an excess of Xe-129 derived from I-129. Both meteorites show significant variations in the composition of the spallation Xe attributable to the separation of the Ba and REE components. The Ba-related spallation in Lewis Cliff differs from that in Angra dos Reis primarily in a lower relative yield of the neutron-sensitive Xe-131 isotope, suggesting a lower neutron flux during cosmic ray exposure for the Lewis Cliff meteorite.

Hohenberg, Charles M.↗

Iodine-xenon, chemical, and petrographic studies of Semarkona chondrules - Evidence for the timing of aqueous alteration

The relationship of the I-Xe system of the Semarkona meteorite to other measured properties is investigated via INAA, petrographic, and noble-gas analyses on 17 chondrules from the meteorite. A range of not less than 10 Ma in apparent I-Xe ages is observed. The three latest apparent ages fall in a cluster, suggesting the possibility of a common event. It is argued that the initial I-129/I-127 ratio (R0) is related to chondrule type and/or mineralogy, with nonporphyritic and pyroxene-rich chondrules showing evidence for lower R0s than porphyritic and olivine-rich chondrules. Chondrules with sulfides on or near the surface have lower R0s than other chondrules. The He-129/Xe-132 ratio in the trapped Xe component anticorrelates with R0, consistent with the evolution of a chronometer in a closed system or in multiple systems. It is concluded that the variations in R0 represent variations in ages, and that later events, possibly aqueous alteration, preferentially affected chondrules with nonporphyritic textures and/or sulfide-rich exteriors about 10 Ma after the formation of the chondrules.

Swindle, T. D.↗

An NMR Study of Microvoids in Polymers

An understanding of polymer defect structures, like microvoids in polymeric matrices, is most crucial to their fabrication and application potential. In this project guest atoms are introduced into the microvoids in PMR-15 and NMR is used to determine microvoid sizes and locations. Xenon is a relatively inert probe that would normally not be found naturally in polymer or in NMR probe materials. There are two NMR active Xenon isotopes, Xe-129 and Xe-131. The Xe atom has a very high polarizability, which makes it sensitive to the intracrystalline environment of polymers. Interactions between the Xe atoms and the host matrix perturb and Xe electron cloud, deshielding the nuclei, and thereby expanding the range of the observed NMR chemical shifts. This chemical shift range which may be as large as 5000 ppm, permits subtle structural and chemical effects to be studied with high sensitivity. The Xe-129-NMR line shape has been found to vary in response to changes in the pore symmetry of the framework hosts in Zeolites and Clathrasil compounds. Before exposure to Xe gas, the PMR-15 samples were dried in a vacuum oven at 150 C for 48 hours. The samples were then exposed to Xe gas at 30 psi for 72 hours and sealed in glass tubes with 1 atmosphere of Xenon gas. Xenon gas at 1 atmosphere was used to tune up the spectrometer and to set up the appropriate NMR parameters. A series of spectra were obtained interspersed with applications of vacuum and heating to drive out the adsorbed Xe and determine the role of Xe-Xe interactions in the observed chemical shift.

Toy, James↗

X-Ray Continua of Broad Absorption Line Quasars

The targets for this program, PG1416-129 and LBQS 2212-1759 were known to be Broad Absorption Line Quasars (BALQSOs). BALQSOs are highly absorbed in soft X-rays. Good high energy response of Rossi-XTE made them ideal targets for observation. We observed LBQS 2212-1759 with PCA. We have now analyzed the data and found that the source was not detected. Since our target was expected to be faint, reliable estimate of background was very important. With the release of new FTOOLS (version 4.1) we were able to do so. We also analyzed a well known bright object and verified our results with the published data. This gave us confidence in the non-detection of our target LBQS 2212-1759. We are currently investigating the implications of this non-detection. Due to some scheduling problems, our second target PG1416-129 was not observed in A01. It was observed on 06/26/98. This target was detected with RXTE. We are now working on the spectral analysis with XSPEC.

Mathur, S.↗

Iodine-Xenon Dating: Sensitive Chronometer for Reprocessing in the Primitive Solar System

The I-Xe chronometer is based upon decay of I-129 to Xe-129 in the early Solar System. Recent comparison of I-Xe system in individual mineral separates from twelve different meteorites with independent Pb-Pb data has demonstrated that I-Xe clock is a reliable sensitive chronometer when applied to a single mineral system. Since most iodine hosts are secondary minerals, the I-Xe clock generally records post-formational processing, providing the information on early meteorite evolution. Absolute I-Xe ages can be found by normalization using the measured I-Xe and Pb-Pb ages of Acapulco phosphate (4.557 plus or minus 0.002 Ga). Absolute ages for the I-Xe internal standards Shallow water and Bjurbole, 4.566 plus or minus 0.002 Ga and 4.565 plus or minus 0.003 Ga, respectively, provide absolute I-Xe ages for all other samples. The I-Xe age of bulk meteorite is meaningful and interpretable only when the carrier of primordial iodine is a major mineral phase (e. g., enstatite chondrites). Using the "monomineral" approach, separated phases from the Richardton H5 chondrite provide a case history of post-formational alteration in this object. This work applies the I-Xe chronometer to determine the times of reprocessing of selected minerals in single meteorite types. A preliminary account of this work was recently reported. Additional information is contained in the original extended abstract.

Pravdivtseva, O. V.↗

Biomedical Investigations with Laser-Polarized Noble Gas Magnetic Resonance

We are developing laser-polarized noble gas nuclear magnetic resonance (NMR) as a novel biomedical imaging tool for ground-based and eventually space-based application. This emerging multidisciplinary technology enables high-resolution gas-space magnetic resonance imaging (MRI) (e.g., of lung ventilation) as well as studies of tissue perfusion. In addition, laser-polarized noble gases (He-3 and Xe-129) do not require a large magnetic field for sensitive detection, opening the door to practical MRI at very low magnetic fields with an open, lightweight, and low-power device. We are pursuing two specific aims in this research. The first aim is to develop a low-field (< 0.01 T) instrument for noble gas MRI of humans, and the second aim is to develop functional MRI of the lung using laser-polarized Xe-129 and related techniques.

Walsworth, Ronald L.↗

Ar-Ar and I-Xe Ages and the Thermal History of IAB Meteorites

Studies of several samples of the large Caddo County IAB iron meteorite reveal andesitic material, enriched in Si, Na, Al and Ca, which is essentially unique among meteorites. This material is believed to have formed from a chondritic source by partial melting and to have further segregated by grain coarsening. Such an origin implies extended metamorphism of the IAB parent body. New Ar-39- Ar-40 ages for silicate from three different Caddo samples are consistent with a common age of 4.50-4.51 Gyr ago. Less well defined Ar-Ar degassing ages for inclusions from two other IABs, EET8333 and Udei Station, are approx.4.32 Gyr, whereas the age for Campo del Cielo varies considerably over approx.3.23-4.56 Gyr. New I-129-Xe-129 ages for Caddo County and EET8333 are 4557.9+/-0.1 Myr and 4557-4560 Myr, respectively, relative to an age of 4562.3 Myr for Shallowater. Considering all reported Ar-Ar degassing ages for IABs and related winonaites, the range is approx.4.32-4.53 Gyr, but several IABs give similar Ar ages of 4.50-4.52 Gyr. We interpret these older Ar ages to represent cooling after the time of last significant metamorphism on the parent body, and the younger ages to represent later 40Ar diffusion loss. The older Ar-Ar ages for IABs are similar to Sm-Nd and Rb-Sr isochron ages reported in the literature for Caddo County. Considering the possibility that IAB parent body formation was followed by impact disruption, reassembly, and metamorphism (e.g., Benedix et al. 2000), the Ar-Ar ages and IAB cooling rates deduced from Ni concentration profiles in IAB metal (Herpfer et al., 1994) are consistent if the time of the post-assembly metamorphism was as late as approx.4.53 Gyr ago. However, I-Xe ages reported for some IABs define much older ages of approx.4558-4566 Myr, which cannot easily be reconciled with the much younger Ar-Ar and Sm-Nd ages. An explanation for the difference in radiometric ages of IABs may reside in combinations of the following: a) I-Xe ages have very high closure temperatures and were not reset during metamorphism approx.4.53 Gyr ago; b) a bias exists in the 40K decay constants which makes these Ar-Ar ages approx.30 Myr too young; c) the reported Sm-Nd and Rb-Sr ages for Caddo are in error by amounts equal to or exceeding their reported 2-sigma uncertainties; and d) about 30 Myr after the initial heating that produced differentiation of Caddo silicate and mixing of silicate and metal, a mild metamorphism of the IAB parent body reset the Ar-Ar ages.

Bogard, Donald D.↗

Ar-Ar and I-Xe Ages and the Thermal History of IAB Meteorites

Studies of several samples of the large Caddo County IAB iron meteorite reveal andesitic material, enriched in Si, Na, Al and Ca, which is essentially unique among meteorites. This material is believed to have formed from a chondritic source by partial melting and to have further segregated by grain coarsening. Such an origin implies extended metamorphism of the IAB parent body. New Ar-39-Ar-40 ages for silicate from three different Caddo samples are consistent with a common age of 4.50-4.51 Gyr ago. Less well defined Ar-Ar degassing ages for inclusions from two other IABs, EET8333 and Udei Station, are approx.4.32 Gyr, whereas the age for Campo del Cielo varies considerably over approx.3.23-4.56 Gyr. New I-129-Xe-129 ages for Caddo County and EET8333 are 4561.9+/-0.1 Myr and 4560- 4563 Myr, respectively, relative to an age of 4566 Myr for Shallowater. Considering all reported Ar-Ar ages for IABs and related winonaites, the range is approx.4.32-4.53 Gyr, but several IABs give similar Ar ages of 4.50-4.52 Gyr. We interpret these older ages to represent cooling after the time of last significant metamorphism on the parent body, and the younger ages to represent later Ar-40 diffusion loss. These older Ar-Ar ages are similar to Sm-Nd and Rb-Sr isochron ages reported in the literature for Caddo County. Considering the possibility that IAB parent body formation was followed by impact disruption, reassembly, and metamorphism (e.g., Benedix et al. 2000), the time of the post-assembly metamorphism may have been as late as approx.4.53 Gyr ago. However, precise I-Xe ages reported for some IABs define a range of ages of approx.4560 to approx.4576 Myr. The older I-Xe ages exceed the oldest precise radiometric ages of meteorites, appear unrealistic, and s,uggest a bias in the calibration of all I-Xe ages. But even with such a bias, the I-Xe ages of IABs cannot easily be reconciled with the much younger Ar-Ar and Sm-Nd ages and with cooling rates deduced from Ni concentration profiles in IAB metal (Herpfer et al., 1994). An explanation for the difference in radiometric ages of IABs may reside in combinations of the following: a) I-Xe ages have very high closure temperatures and were not reset during metamorphism; b) a bias exists in the K-40 decay constants; c) the reported Sm-Nd and Rb-Sr ages for Caddo are in error by amounts equal to or exceeding their reported 2-sigma uncertainties; and 4) the IAB parent body may have experienced a mild metamorphism approx.30 Myr after the initial heating that produced differentiation of Caddo silicate and mixing of silicate and metal.

Bogard, Donald D.↗

Ar-Ar and I-Xe Ages and the Thermal History of IAB Meteorites

Studies of several samples of the large Caddo County IAB iron meteorite reveal andesitic material, enriched in Si, Nay Al and Ca, which is essentially unique among meteorites. This material is believed to have formed from a chondritic source by partial melting and to have further segregated by grain coarsening. Such an origin implies extended metamorphism of the IAB parent body. New Ar-39-Ar-40 ages for silicate from three different Caddo samples are consistent with a common age of 4.50- 4.51 Gyr ago. Less well defined Ar-Ar degassing ages for inclusions from two other IABs, EET8333 and Udei Station, are approx.4.32 Gyr, whereas the age for Campo del Cielo varies considerably over approx.3.23-4.56 Gyr. New I-129-Xe-129 ages for Caddo County and EET8333 are 4561.9 +/-0.1 Myr and 4560-4563 Myr, respectively, relative to an age of 4566 Myr for Shallowater. Considering all reported Ar-Ar ages for IABs and related winonaites, the range is approx.4.32-4.53 Gyr, but several IABs give similar Ar ages of 4.50-4.52 Gyr. We interpret these older ages to represent cooling after the time of last significant metamorphism on the parent body, and the younger ages to represent later Ar-40 diffusion loss. These older Ar-Ar ages are similar to Sm-Nd and Rb-Sr isochron ages reported in the literature for Caddo County. Considering the possibility that IAB parent body formation was followed by impact disruption, reassembly, and metamorphism (e.g., Benedix et al. 2000), the time of the post-assembly metamorphism may have been as late as approx.4.53 Gyr ago. However, precise I-Xe ages reported for some IABs define a range of ages of approx.4560 to approx.4576 My. The older I-Xe ages exceed the oldest precise radiometric ages of meteorites, appear unrealistic, and suggest a bias in the calibration of all I-Xe ages. But even with such a bias, the I-Xe ages of IABs cannot easily be reconciled with the much younger Ar-Ar and Sm-Nd ages and with cooling rates deduced from Ni concentration profiles in IAB metal (Herpfer et al., 1994). An explanation for the difference in radiometric ages of IABs may reside in combinations of the following: a) I-Xe ages have very high closure temperatures and were not reset during metamorphism; b) a bias exists in the K-40 decay constants; c) the reported Sm-Nd and Rb-Sr ages for Caddo are in error by amounts equal to or exceeding their reported 2-sigma uncertainties; and 4) the IAB parent body may have experienced a mild metamorphism approx.30 Myr after the initial heating that produced differentiation of Caddo silicate and mixing of silicate and metal. 129 129

Bogard, Donald D.↗

Ar-Ar and I-XE Ages and the Thermal History of IAB Meteorites

Studies of several samples of the large Caddo County IAB iron meteorite reveal andesitic material, enriched in Si, Na, Al and Ca which is essentially unique among meteorites. This material is believed to have formed from a chondritic source by partial melting and to have further segregated by grain coarsening. Such an origin implies extended metamorphism of the IAB parent body. New Ar-39- Ar-40 ages for silicate from three different Caddo samples are consistent with a common age of 4.50- 4.51 Gyr ago. Less well defined Ar-Ar degassing ages for inclusions from two other IABs, EET8333 and Udei Station, are approx. 4.32 Gyr, whereas the age for Campo del Cielo varies considerably over approx. 3.23-4.56 Gyr. New I-129-Xe-129 ges for Caddo County and EET8333 are 4561.9 plus or minus 0.1 Myr and 4560-4563 Myr, respectively, relative to an age of 4566 Myr for Shallowater. Considering all reported Ar-Ar ages for IABs and related winonaites, the range is approx. 4.32-4.53 Gyr, but several IABs give similar Ar ages of 4.50-4.52 Gyr. We interpret these older ages to represent cooling after the time of last significant metamorphism on the parent body, and the younger ages to represent later 40Ar diffusion loss. These older Ar-Ar ages are similar to Sm-Nd and Rb-Sr isochron ages reported in the literature for Caddo County. Considering the possibility that IAB parent body formation was followed by impact disruption, reassembly, and metamorphism (e.g., Benedix et al. 2000), the time of the postassembly metamorphism may have been as late as approx. 4.53 Gyr ago. However, precise I-Xe ages reported for some IABs define a range of ages of approx. 4560 to approx. 4576 Myr. The older I-Xe ages exceed the oldest precise radiometric ages of meteorites, appear unrealistic, and suggest a bias in the calibration of all I-Xe ages. But even with such a bias, the I-Xe ages of IABs cannot easily be reconciled with the much younger Ar-Ar and Sm-Nd ages and with cooling rates deduced from Ni concentration profiles in IAB metal (Herpfer et al., 1994). An explanation for the difference in radiometric ages of IABs may reside in combinations of the following: a) I-Xe ages have very high closure temperatures and were not reset during metamorphism; b) a bias exists in the K-40 decay constants; c) the reported Sm-Nd and Rb-Sr ages for Caddo are in error by amounts equal to or exceeding their reported 2-sigma uncertainties; and 4) the IAB parent body may have experienced a mild metamorphism approx.30 My after the initial heating that produced differentiation of Caddo silicate and mixing of silicate and metal.

Bogard, Donald D.↗

Post-Flight Microbial Analysis of Samples from the International Space Station Water Recovery System and Oxygen Generation System

The Regenerative, Environmental Control and Life Support System (ECLSS) on the International Space Station (ISS) includes the the Water Recovery System (WRS) and the Oxygen Generation System (OGS). The WRS consists of a Urine Processor Assembly (UPA) and Water Processor Assembly (WPA). This report describes microbial characterization of wastewater and surface samples collected from the WRS and OGS subsystems, returned to KSC, JSC, and MSFC on consecutive shuttle flights (STS-129 and STS-130) in 2009-10. STS-129 returned two filters that contained fluid samples from the WPA Waste Tank Orbital Recovery Unit (ORU), one from the waste tank and the other from the ISS humidity condensate. Direct count by microscopic enumeration revealed 8.38 x 104 cells per mL in the humidity condensate sample, but none of those cells were recoverable on solid agar media. In contrast, 3.32 x lOs cells per mL were measured from a surface swab of the WRS waste tank, including viable bacteria and fungi recovered after S12 days of incubation on solid agar media. Based on rDNA sequencing and phenotypic characterization, a fungus recovered from the filter was determined to be Lecythophora mutabilis. The bacterial isolate was identified by rDNA sequence data to be Methylobacterium radiotolerans. Additional UPA subsystem samples were returned on STS-130 for analysis. Both liquid and solid samples were collected from the Russian urine container (EDV), Distillation Assembly (DA) and Recycle Filter Tank Assembly (RFTA) for post-flight analysis. The bacterium Pseudomonas aeruginosa and fungus Chaetomium brasiliense were isolated from the EDV samples. No viable bacteria or fungi were recovered from RFTA brine samples (N= 6), but multiple samples (N = 11) from the DA and RFTA were found to contain fungal and bacterial cells. Many recovered cells have been identified to genus by rDNA sequencing and carbon source utilization profiling (BiOLOG Gen III). The presence of viable bacteria and fungi from WRS and OGS subsystems demonstrates the need for continued monitoring of ECLSS during future ISS operations and investigation of advanced antimicrobial controls.

Birmele, Michele N.↗

Development of a Conditioned System-Level Groundwater Model to Evaluate Long-Term Groundwater Impacts within a Performance Assessment - 20115

A preliminary performance assessment (PA) of single-shell tank Waste Management Area (WMA) A-AX located at the U.S. Department of Energy (DOE)'s Hanford Site in southeastern Washington is being conducted to satisfy the requirements of DOE Order 435.1 [1] as it relates to closure of the single-shell radioactive waste tanks in the WMA A-AX tank farms. A PA assesses the fate, transport, and impacts of radionuclides within a low-level radioactive waste disposal facility in its assumed closure configuration and the subsequent potential doses to humans over a 1,000-year compliance period and a 10,000-year performance evaluation period. The WMA A-AX preliminary PA evaluation is structured around the complementary use of process-level and system-level models to calculate the facility performance against established DOE Order 435.1 [1] performance objectives. Process-level models are those that represent a detailed phenomenological representation of processes of concern in the PA. Process models typically only represent one or a few of the components of the PA, such as groundwater flow and transport, and must be integrated with other modeling elements to perform PA calculations. System-level models are those that are abstracted from the process models, retaining the essential features of the process model, while allowing integration of all aspects of the PA in a single modeling framework. System-level models are often characterized by coarser numerical discretization, lower dimensionality, or other similar simplifications compared to the process-level model. Traditionally, a three-dimensional (3-D) process-level model is utilized primarily to evaluate the long-term impact on groundwater and the potential doses to individuals who consume contaminated groundwater. System-level models are also utilized to evaluate the groundwater pathway in PAs. These models typically have reduced dimensionality (1-D) and are conditioned utilizing flow fields (Darcy fluxes) and moisture content distributions that are abstracted from the process level models. The abstraction approach assures that the flow field in both models is consistent for a specific set of input parameters for flow, differing only in the discretization and dimensionality of the two models. The preliminary WMA A-AX PA incorporates a detailed representation of the geological system and hydraulic properties within the 3-D model STOMP{sup C} numerical code so that the effects of relevant features and processes on water flow and radionuclide transport in the subsurface can be evaluated. The complementary system-level model is developed utilizing the GoldSim{sup C} code to implement a simplified, 1-D equivalent model to represent the groundwater pathway. Contaminant transport through the vadose zone and unconfined aquifer for Tc-99 and I-129 were evaluated in each of the models. Adjustments to the saturated portion of the GoldSim{sup C} 1-D model were required to mimic the dispersion effect captured with the 3-D STOMP{sup C} model. Once this conditioning was conducted, highly similar results for the transport of Tc-99 and I-129 were achieved at the point of calculation, located 100 m downgradient from the WMA A-AX fenceline. These radionuclides represent elements that are regarded as primary dose drivers in the PA groundwater pathway analysis. The high degree of conformance between the two models suggests that the use of the equivalent 1-D system model is suitable for evaluating the full suite of radionuclides that will be released from the tank sources within WMA A-AX over the 1,000-year compliance period and over the 10,000-year evaluation period. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Iodine Air Sampling: Installation and Preliminary Results

The F-Area wetlands are a known sink for radioiodine generated at the Savannah River Site (SRS). Wastewater containing iodine-129 ( 129 I) was discharged into the F-Area Seepage Basins for disposal, but the acidity of the wastewater mobilized some of the contaminants from the basin soil through the vadose zone and into the groundwater; ultimately creating a groundwater plume that extends towards Fourmile Branch and its associated wetland areas. Dissolved radioiodine specifically has migrated to the nearby F-Area wetlands, where it persists as a contaminant of concern. Accumulation and resurfacing of 129 I in the wetlands and nearby areas creates a potential secondary source zone where changes in biogeochemical conditions could result in the release of this sequestered 129 I to the air. Monitoring data has indicated that 129 I has a seasonal behavior at several surface water stations, with high concentrations during summertime and low concentrations during wintertime. Still, it is not known which factors control the seasonal behavior of 129 I. Further, it has been reported that 129 I contributed approximately 23% to the 2019 SRS offsite air pathway dose to the representative person for that year (SRNS, 2020), but air measurements of 129 I have never been taken in the F-Area wetlands. Because air emissions of 129 I from the wetlands have never been investigated, it is not known if this could be a potential release pathway that needs to be included in the site conceptual model. To address these unknowns, the Savannah River National Laboratory (SRNL) has an applied research task to investigate whether 129 I in the wetlands is emitted to the air and, if so, whether air concentrations exhibit seasonal variation. This report presents information about the system recently installed in the F-Area wetlands for measuring 129 I, as well as analysis results for samples collected June through August 2023. Quantification of this constituent will provide a better understanding of the contribution of airborne 129 I from the F-Area wetlands to the offsite dose and better inform ongoing and future remedial actions.

54 ENVIRONMENTAL SCIENCES↗

Sol–gel synthesis of iodosodalite precursors and subsequent consolidation with a glass binder made from oxides and sol–gel routes

Radioiodine accumulates in aqueous solutions and off-gas streams during nuclear fuel reprocessing due to its solubility in aqueous solutions and volatility, respectively. Additionally, radioiodine is highly mobile in geological environments and iodine-129 has been found to be one of the largest long-term contributors to chronic dose to humans in scenarios of radionuclide migration from geological repositories. Most of the radioiodine can be captured during fuel reprocessing in off-gas streams using solid sorbents and scrubbing solutions. Once iodine is captured, it must be stored in a durable form for eventual disposal. Iodosodalite has been investigated as a waste form for radioiodine, however these synthesis processes typically result in mixed products and iodine volatilization during consolidation. Therefore, this paper proposes a novel approach to synthesizing iodosodalite utilizing a sol-gel method. This method was chosen to lower processing temperatures and improve product yield. Preliminary experiments conducted to determine the viability of this synthetic method are presented. Additionally, consolidation of sol-gel derived iodosodalite with a glass-binder was explored using three different methods: 1) incorporating the glass-binder during gel preparation using alkoxide precursors; 2) separately preparing the glass binder using a sol-gel method; and 3) separately preparing the glass-binder using a melt-quench technique. Glass-bonded iodosodalite was successfully synthesized using these novel sol-gel approaches.

36 MATERIALS SCIENCE↗

The simultaneous removal of technetium and iodine from Hanford tank waste

The simultaneous removal of radionuclides technetium-99 and iodine-129 from an actual decontaminated Hanford tank waste sample (a mixture of decontaminated waste from tanks 241-AP-105 and 241-AP-107) was demonstrated for the first time in this work. A series of commercially available ion exchange resins were evaluated in batch contact tests in the tank waste, and all showed removal of both Tc and I. The highest Tc removal was observed for Purolite A530e while the highest iodine removal was observed for ResinTech SIR-110-MP. Batch tests in simulated tank waste with these two resins showed that the SIR-110-HP-MP had consistently higher K d for both pertechnetate and iodide and much higher K d than previous works on Tc removal from Hanford waste. As such, the SIR-110-MP was evaluated in a dual -column (lead/lag) test processing 5.2L of the tank waste mixture showing 60% breakthrough of Tc on the lead column and no significant breakthrough on the lag after 625 bed volumes (BV, 6 mL size) while significant iodine breakthrough (>50%) occurred after 28 BV. The limited iodine uptake was attributed to the column conditions generating mass transfer limitations. A fraction of the Tc and I was not captured by the resin (<10%) in either the batch tests or column tests. The iodine fraction was identified to be an iodide, likely organo-iodide. The fraction of the Tc was identified as a non-pertechnetate species, which is the first time non-pertechnetate has been identified in AP-105 and AP-107 tanks, although the exact species is still unknown.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗