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Ion Exchange Processing of AW-105 Hanford Tank Waste through Crystalline Silicotitanate in a Staged 2- then 3-Column System
The Hanford Site stores an estimated 56 million gallons of mixed radioactive and chemically hazardous waste in large underground tanks. In support of the Direct Feed Low-Activity Waste (DFLAW) Program for expediting Hanford tank waste supernate treatment, laboratory-scale ion exchange processing using prototypic unit operations was conducted on AW-105 tank waste at the Pacific Northwest National Laboratory Radiochemical Processing Laboratory. This report describes the small-scale ion exchange testing with 9.2 L of diluted and filtered supernate from Tank 241-AW-105 (hereafter referred to as AW-105) at 16 °C (62 °F). One of the waste acceptance criteria (WAC) for the Waste Treatment Plant (WTP) Low-Activity Waste Facility is that the waste must contain less than 3.18×10 -5 Ci 137 Cs per mole of Na. For the AW-105 tank waste to meet this criterion, only 0.225% of the influent 137 Cs concentration may be delivered to the WTP; this requires a Cs decontamination factor of 445. Testing with AW-105 matched current Tank Side Cesium Removal (TSCR) facility prototypic operations where a lead-lag configuration was used until the lag column reached the WAC limit, then a polish column was brought online for continued processing in a lead-lag-polish column configuration. Feed was processed at 1.9 bed volumes (BVs) per hour; the flowrate, in terms of contact time with the crystalline silicotitanate (CST) bed, matched the expected flowrate at TSCR. The Cs-decontaminated product was retained for vitrification testing (to be reported separately). The lead column reached 83% Cs breakthrough after processing ~1500 BVs of feed; the 50% Cs breakthrough was interpolated from the breakthrough data and occurred at 1041 BVs. Despite the AW-105 having a significantly higher K concentration (0.55 M compared to 0.10 M), testing compared to previous AP-107 ion exchange column testing at 16 °C showed no difference in BVs processed to reach the WAC on the lead column and only an approximate ~20 BV decrease in volume processed to reach the WAC limit on the lag column. The negligible differences in capacity despite the 5x concentration differences in K was determined to be due to the significantly lower NO3 concentration in the AW-105 supernate compared to the AP-107 tank waste matrix. A comparison in breakthrough curves for the two tests also indicated slightly faster kinetic behavior in the AW-105, with the variations in feed matrices (lower NO3 concentration) likely responsible for the deviation. The Cs effluent from the lag column reached the WAC limit after processing 772 BVs. Anticipating this breakthrough point, the polish column was preemptively installed around 675 BVs. Cs breakthrough from the lag column began at 300 BVs, reaching 1.10×10 1 µCi/mL, or 14.13 % Cs breakthrough, after processing all 1500 BVs of feed. The polish column processed nominally 830 BVs and reached 2.10×10 -1 µCi/mL, or 0.27 % Cs breakthrough at the conclusion of the test. Table S.1 and Figure S.1 summarize the observed column performance and relevant Cs loading characteristics.
Filtration of Hanford Tank 241-AW-105 Supernatant at 16 °C
Approximately 9 L of supernatant from Hanford waste tank 241-AW-105 was delivered by Hanford Tank Waste Operations and Closure (H2C) to the Radiochemical Processing Laboratory (RPL) at Pacific Northwest National Laboratory (PNNL). The thirty-six 241-AW-105 sample bottles consisted of four sets of nine samples, with each set pulled from a unique tank sampling level. Prior to testing, samples from each level were composited and diluted to 5.5 M Na to provide nominally level-independent feed for dead-end filtration and ion exchange testing. The composited 241-AW-105 supernatant was chilled to 16 °C for 1 week prior to testing. Filtration testing was then conducted using a backpulse dead-end filter (BDEF) system equipped with a feed vessel and a Mott inline filter (Model 6610, Media Grade 5) in the hot cells of the RPL. The purpose of this testing was to (a) demonstrate dead-end filtration (DEF) of 241-AW-105 feed at reduced temperature to obtain prototypic Tank Side Cesium Removal (TSCR) flux rates and identify issues that may impact filtration after dilution to 5.5 M Na, and (b) provide feed for follow-on ion exchange unit operation. The feed was filtered through the BDEF system at a targeted flux of 0.065 gpm/ft2. For most of the filtration campaign, the differential pressure required to effect filtration at 0.065 gpm/ft2 was slow to increase. After all the feed bottles had been pumped into the slurry reservoir, the bottoms of the bottles were added to the reservoir and transmembrane pressure (TMP) reached 2.0 psid (the TSCR action limit). A backpulse was performed after >50 hours of filtration to remove fouled solids and reduce the TMP. The filter was cleaned after completing filtration of the 241-AW-105 feed, and clean water flux tests showed filter performance was effectively restored. Solids concentrated from the backpulse solutions were composed of steel-like particles, uranium-bearing phases, Mn-Fe phases, a Ce-bearing phase, Zr phases, and some smaller Ca-bearing particles. The Ca-bearing and U bearing phases were identified as calcite and clarkeite, respectively.
Time sequence spectroscopy of AW UMa. The 518 nm Mg I triplet region analyzed with broadening functions
High-resolution spectroscopic observations of AW UMa, obtained on three consecutive nights with a median time resolution of 2.1 minutes, have been analyzed using the broadening function method in the spectral window of 22.75 nm around the 518 nm Mg i triplet region. Doppler images of the system reveal the presence of vigorous mass motions within the binary system; their presence puts into question the solid-body rotation assumption of the contact binary model. AW UMa appears to be a very tight, semi-detached binary; the mass transfer takes place from the more massive to the less massive component. The primary, a fast-rotating star with Vsini=181.4±2.5 km s{sup −1}, is covered with inhomogeneities: very slowly drifting spots and a dense network of ripples more closely participating in its rotation. The spectral lines of the primary show an additional broadening component (called the “pedestal”) that originates either in the equatorial regions, which rotate faster than the rest of the star by about 50 km s{sup −1}, or in an external disk-like structure. The secondary component appears to be smaller than predicted by the contact model. The radial velocity field around the secondary is dominated by accretion of matter transferred from (and possibly partly returned to) the primary component. The parameters of the binary are Asini=2.73±0.11 R{sub ⊙} and M{sub 1}sin{sup 3}i=1.29±0.15 M{sub ⊙}, M{sub 2}sin{sup 3}i=0.128±0.016 M{sub ⊙}. The mass ratio, q{sub sp}=M{sub 2}/M{sub 1}=0.099±0.003, while still the most uncertain among the spectroscopic elements, is substantially different from the previous numerous and mutually consistent photometric investigations which were based on the contact model. It should be studied why photometry and spectroscopy give such discrepant results and whether AW UMa is an unusual object or if only very high-quality spectroscopy can reveal the true nature of W UMa-type binaries.
Dead-End Filtration and Crystalline Silicotitanate Cesium Ion Exchange with Hanford Tank Waste AW-102
The Direct Feed Low-Activity Waste (DFLAW) flowsheet provides for the initial production of immobilized low-activity waste (ILAW) by feeding low-activity waste (LAW) directly from tank farms to the Hanford Tank Waste Treatment and Immobilization Plant (WTP) LAW facility for immobilization. Prior to the transfer of feed to the WTP LAW facility, tank supernatant waste will be pretreated by the Tank Side Cesium Removal (TSCR) system to meet the WTP LAW waste acceptance criteria (<3.18E-5 Ci 137Cs/mole of Na). This pretreatment facility will filter the waste to remove suspended solids and remove cesium from the waste stream through ion exchange. Bench-scale filtration testing of 7.4 liters of diluted of AW-102 supernate was conducted using dead-end filtration in the hot cells of the Radiochemical Processing Laboratory at Pacific Northwest National Laboratory. A Mott 70-mm disc filter (media grade 5) was used to capture solids. The filter area was adjusted to 2.2 in2 to match the planned TSCR supernate process volume to surface area ratio. There was no indication of filter fouling and no recoverable solids were observed on the filter. Ion exchange testing with the filtered, diluted AW-102 supernatant was conducted using crystalline silicotitanate (CST) ion exchange media. The IONSIV R9140-B CST was provided by Honeywell UOP, LLC in 2018 (Lot number 8056202-999). The column testing operations were prototypic to the intended Low-Activity Waste Pretreatment System operations in a lead-lag column format, although on a small-scale basis with 10-mL CST beds. The feed was processed downflow through the lead column and then through the lag column at ~1.8 bed volumes per hour (BV/h). After 88.6 BVs of feed processing, the volume in the feed bottle dropped below the inlet tube and the lead column fluid headspace was displaced with air. Feed processing was suspended while a new column was prepared and installed into the lead position. A total of 450 BVs of diluted AW-102 feed were processed through the new lead column; only 4.3% Cs breakthrough was achieved. This volume of feed was insufficient to generate useful Cs loading information without extrapolation. A straight-line extrapolation was used to determine the 50% breakthrough of the lead column and contract limit breakthrough from the lag. The values were found to be 1200 BVs and 930 BVs, respectively.
Vitrification of Hanford Tank 241-AW-105 Waste and Equivalent Simulant
Hanford Site nuclear waste is to be vitrified at the Waste Treatment and Immobilization Plant (WTP), which is a part of the safe and efficient retrieval, treatment, and disposal mission of the U.S. Department of Energy - Hanford Field Office. A portion of Hanford tank 241-AW-105 (referred to herein as AW-105) waste was retrieved by Hanford Tank Waste Operations and Closure (H2C) and transferred to Pacific Northwest National Laboratory (PNNL). Compared to previously received and vitrified wastes (AP-107, AP-101, AN-107 and AP-105), the concentration of potassium in AW-105 was greater by an order of magnitude.
Investigation of Tank 241-AW-104 Composite Floating Layer
Seven grab samples and one field blank were taken from Tank 241-AW-104 (AW-104) on June 2, 2017, and received at 222-S Laboratory on June 5, 2017. A visible layer with brown solids was observed floating on the top of two surface tank waste samples (4AW-17-02 and 4AW 17 02DUP). The floating layer from both samples was collected, composited, and submitted for chemical analyses and solid phase characterization in order to understand the composition of the floating layer. Tributyl phosphate and tridecane were higher in the floating layer than in the aqueous phase. Density in the floating layer was slightly lower than the mean density of all grab samples. Sodium nitrate and sodium carbonate were major components with a trace of gibbsite and very small size agglomerates were present in the solids of the floating layer. The supernate consisted of organics, soluble salt, and particulates.
High-quality permanent draft genome sequence of the extremely osmotolerant diphenol degrading bacterium Halotalea alkalilenta AW-7T, and emended description of the genus Halotalea
Members of the genus Halotalea (family Halomonadaceae) are of high significance since they can tolerate the greatest glucose and maltose concentrations ever reported for known bacteria and are involved in the degradation of industrial effluents. Here, the characteristics and the permanent-draft genome sequence and annotation of Halotalea alkalilenta AW-7T are described. The microorganism was sequenced as a part of the Genomic Encyclopedia of Type Strains, Phase I: the one thousand microbial genomes (KMG) project at the DOE Joint Genome Institute, and it is the only strain within the genus Halotalea having its genome sequenced. The genome is 4,467,826 bp long and consists of 40 scaffolds with 64.62 % average GC content. A total of 4,104 genes were predicted, comprising of 4,028 protein-coding and 76 RNA genes. Most protein-coding genes (87.79 %) were assigned to a putative function. Halotalea alkalilenta AW-7T encodes the catechol and protocatechuate degradation to β-ketoadipate via the β-ketoadipate and protocatechuate ortho-cleavage degradation pathway, and it possesses the genetic ability to detoxify fluoroacetate, cyanate and acrylonitrile. Lastly, an emended description of the genus Halotalea Ntougias et al. 2007 is also provided in order to describe the delayed fermentation ability of the type strain.
Analysis of Respirator Cartridge Performance Testing on a Hanford AW Tank Farm Exhauster Slipstream
Washington River Protection Solutions (WRPS) conducted tests on two types of chemical cartridges for use in air-purifying respirators (APR) to determine the period of time that the cartridges would provide adequate performance for APRs used to protect workers when exposed to a mixture of Chemicals of Potential Concern (COPCs) from vapors exiting the exhauster for the Hanford AW tank farm. The Occupational Safety and Health Administration (OSHA) identifies cartridge testing as a valid approach for establishing a cartridge change schedules. Testing is commonly applied in situations where mixtures of COPCs exist, and where other approaches, such as manufacturer recommendations and modeling, are less reliable. The tests were designed and conducted to assure measurement and/or control of the key variables OSHA identified as important to estimate cartridge service-life, including temperature, humidity, COPC concentration, breathing rate, and cartridge adsorption capacity. Testing was conducted from September 23-25, 2016, on a slipstream from the AW exhauster, under static conditions fed to a respirator cartridge test stand developed by WRPS in collaboration with HiLine Engineering (Richland, Washington). Multipurpose respirator cartridges, SCOTT 7422-SD1 and SCOTT 7422-SC1 (SCOTT Safety, Monroe, North Carolina), were assessed on separate days. Sample media (sorbent tubes) were used to collect samples of the vapor stream entering and exiting the respirator cartridge, and were subsequently analyzed for COPC concentrations. Pacific Northwest National Laboratory was tasked with conducting an independent analysis of the analytical results and making recommendations based on the results for respiratory cartridge performance and service life.
Effect of Shielding Gas on the Properties of AW 5083 Aluminum Alloy Laser Weld Joints
The paper deals with the evaluation of the shielding gas influence on the properties of AW 5083 aluminum alloy weld joints produced with disk laser. Butt weld joints were produced under different shielding gas types, namely Ar, He, Ar + 5 vol.% He, Ar + 30 vol.% He and without shielding weld pool. Light and electron microscopy, computed tomography, microhardness measurements and tensile testing were used for evaluation of weld joint properties. He-shielded weld joints were the narrowest ones. On the other hand, Ar-shielded weld joints exhibited largest weld width. The choice of shielding gas had significant influence on the porosity level of welds. The lowest porosity was observed in weld joint produced in Ar with the addition of 5 vol.% He shielding atmosphere (only 0.03%), while the highest level of porosity was detected in weld joint produced in pure He (0.24%). Except unshielded aluminum alloy weld joint, the lowest tensile strength was recorded in He-shielded weld joints. On the contrary, the highest average microhardness was measured in He-shielded weld joints.
Chemical intuition for high thermoelectric performance in monolayer black phosphorus, α-arsenene and aW-antimonene
Identifying materials with intrinsically high thermoelectric performance remains a challenge even with the aid of a high-throughput search. Here, using a chemically intuitive approach based on the bond-orbital theory, three anisotropic 2D group-V materials (monolayer black phosphorus, α-arsenene, and aW-antimonene) are identified as candidates for high thermoelectric energy conversion efficiency. Concepts, such as bond length, bond angle, and bond strength, are used to explain the trends in their electronic properties, such as the band gap and the effective mass. Our first principles calculations confirm that high carrier mobilities and large Seebeck coefficients can be obtained at the same time in these materials, due to complex Fermi surfaces originating from the anisotropic structures. An intuitive understanding of how the bonding character affects phonon transport is also provided with emphasis on the importance of bonding strength and bond anharmonicity. High thermoelectric performance is observed in these materials. In conclusion, our approach provides a powerful tool to identify new thermoelectric materials and evaluate their transport properties.
Mycorrhizal phenotypes and the L aw of the M inimum
Summary Mycorrhizal phenotypes arise from interactions among plant and fungal genotypes and the environment. Differences in the stoichiometry and uptake capacity of fungi and plants make arbuscular mycorrhizal ( AM ) fungi inherently more nitrogen (N) limited and less phosphorus (P) limited than their host plants. Mutualistic phenotypes are most likely in P‐limited systems and commensal or parasitic phenotypes in N‐limited systems. Carbon (C) limitation is expected to cause phenotypes to shift from mutualism to commensalism and even parasitism. Two experiments compared the influence of fertilizer and shade on mycorrhizas in A ndropogon gerardii across three naturally N‐limited or P‐limited grasslands. A third experiment examined the interactive effects of N and P enrichment and shade on A . gerardii mycorrhizas. Our experiments generated the full spectrum of mycorrhizal phenotypes. These findings support the hypothesis that mutualism is likely in P‐limited systems and commensalism or parasitism is likely in N‐limited systems. Furthermore, shade decreased C‐assimilation and generated less mutualistic mycorrhizal phenotypes with reduced plant and fungal biomass. Soil fertility is a key controller of mycorrhizal costs and benefits and the L aw of the M inimum is a useful predictor of mycorrhizal phenotype. In our experimental grasslands arbuscular mycorrhizas can ameliorate P‐limitation but not N‐limitation.
Ecology information request HgC2H6 for 241-AW Tank Farm, 01/13/2015
This information was requested by Phil Gent of Ecology on 12/18/2014 and confirmed on 01/13/2015 to Dale Dyekman.
Investigation of Tank 241-AW-104 Composite Floating Layer
Seven grab samples and one field blank were taken June 2, 2017. A visible layer with brown solids was observed floating on the top of two surface tank waste samples (4AW-17-02 and 4AW 17 02DUP). The floating layers were collected, composited, and submitted for chemical analyses and solid phase characterization in order to understand the composition of the floating layer. Tributyl phosphate and tridecane were higher in the floating layer than in the aqueous phase. Density in the floating layer was slightly lower than the mean density of all grab samples. Sodium nitrate and sodium carbonate were major components with a trace of gibbsite and very small size agglomerates were present in the solids of the floating layer. The supernate consisted of organics, soluble salt, and particulates. These agglomerates include uranium extruded from the supernate by the floating organics.
Automated Particle Analysis of Hanford Tank Wastes 241-AN-106, 241-AN-101, and 241-AW-105
This effort is involved in developing particle size and density distribution (PSDD) for the major phases within Hanford tank waste sludge. The object of this work has been to use automated particle analysis (APA) methods on the Scanning Electron Microscope (SEM) to provide PSDDs. The PSDD can be used to quantify the proportion of gibbsite particles likely to settle quickly and enable blending of wastes that may be prone to pipeline plugging such as the uranium phase, clarkeite with other wastes. The Hanford tank waste solids were analyzed with SEM combined with x-ray Energy Dispersive Spectroscopy (EDS) using APA. This method can allow thousands of individual particles to be characterized and so may provide a more representative view of the samples and information PSDDs. We characterized several as-received sludge samples and developed PSDD with APA. Sample preparation methods were found to impact the collected results, as it was more difficult to collect representative samples of the larger particles. Much of the material was also dried and cemented together that further impacted results.
Three dimensional magnetohydrodynamic simulation of linearly polarised Alfven wave dynamics in Arnold-Beltrami-Childress magnetic field
Previous studies (e.g., Malara et al., Astrophys. J. 533, 523 (2000)) considered small-amplitude Alfven wave (AW) packets in Arnold-Beltrami-Childress (ABC) magnetic field using WKB approximation. They draw a distinction between 2D AW dissipation via phase mixing and 3D AW dissipation via exponentially divergent magnetic field lines. In the former case, AW dissipation time scales as S{sup 1∕3} and in the latter as log(S), where S is the Lundquist number. In this work, linearly polarised Alfven wave dynamics in ABC magnetic field via direct 3D magnetohydrodynamic (MHD) numerical simulation is studied for the first time. A Gaussian AW pulse with length-scale much shorter than ABC domain length and a harmonic AW with wavelength equal to ABC domain length are studied for four different resistivities. While it is found that AWs dissipate quickly in the ABC field, contrary to an expectation, it is found the AW perturbation energy increases in time. In the case of the harmonic AW, the perturbation energy growth is transient in time, attaining peaks in both velocity and magnetic perturbation energies within timescales much smaller than the resistive time. In the case of the Gaussian AW pulse, the velocity perturbation energy growth is still transient in time, attaining a peak within few resistive times, while magnetic perturbation energy continues to grow. It is also shown that the total magnetic energy decreases in time and this is governed by the resistive evolution of the background ABC magnetic field rather than AW damping. On contrary, when the background magnetic field is uniform, the total magnetic energy decrease is prescribed by AW damping, because there is no resistive evolution of the background. By considering runs with different amplitudes and by analysing the perturbation spectra, possible dynamo action by AW perturbation-induced peristaltic flow and inverse cascade of magnetic energy have been excluded. Therefore, the perturbation energy growth is attributed to a new instability. The growth rate appears to be dependent on the value of the resistivity and the spatial scale of the AW disturbance. Thus, when going beyond WKB approximation, AW damping, described by full MHD equations, does not guarantee decrease of perturbation energy. This has implications for the MHD wave plasma heating in exponentially divergent magnetic fields.
An expanded role for the transcription factor WRINKLED1 in the biosynthesis of triacylglycerols during seed development
The transcription factor WRINKLED1 ( WRI1 ) is known as a master regulator of fatty acid synthesis in developing oilseeds of Arabidopsis thaliana and other species. WRI1 is known to directly stimulate the expression of many fatty acid biosynthetic enzymes and a few targets in the lower part of the glycolytic pathway. However, it remains unclear to what extent and how the conversion of sugars into fatty acid biosynthetic precursors is controlled by WRI 1. To shortlist possible gene targets for future in-planta experimental validation, here we present a strategy that combines phylogenetic foot printing of cis-regulatory elements with additional layers of evidence. Upstream regions of protein-encoding genes in A. thaliana were searched for the previously described DNA-binding consensus for WRI1, the ASML1/WRI1 (AW)-box. For about 900 genes, AW-box sites were found to be conserved across orthologous upstream regions in 11 related species of the crucifer family. For 145 select potential target genes identified this way, affinity of upstream AW-box sequences to WRI1 was assayed by Microscale Thermophoresis. This allowed definition of a refined WRI1 DNA-binding consensus. We find that known WRI1 gene targets are predictable with good confidence when upstream AW-sites are phylogenetically conserved, specifically binding WRI1 in the in vitro assay, positioned in proximity to the transcriptional start site, and if the gene is co-expressed with WRI1 during seed development. When targets predicted in this way are mapped to central metabolism, a conserved regulatory blueprint emerges that infers concerted control of contiguous pathway sections in glycolysis and fatty acid biosynthesis by WRI1. Several of the newly predicted targets are in the upper glycolysis pathway and the pentose phosphate pathway. Of these, plastidic isoforms of fructokinase ( FRK 3) and of phosphoglucose isomerase ( PGI 1) are particularly corroborated by previously reported seed phenotypes of respective null mutations.