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At least 1,765 records · Page 98

Raw_data_Batch_I: Ashland Avenue

Date of collection: May 26, 2023 Location: Ashland Avenue, Chicago, IL This data set contains lidar and vision data collected along Ashland Avenue. A south-to-north run starts from the intersection of Irving Park and Ashland and ends at Andersonville Garden. A north-to-south run starts from Andersonville Garden and ends around the intersection of Irving Park and Ashland. The data contains the following Robot Operating System (ROS) topics: - /Central_Camera_blurred – Image flow from coaxial camera heading, vehicle front. - /Left_Camera_blurred – Image flow from left camera, 60° from central camera on the left side. - /Right_Camera_blurred – Image flow from right camera, 60° from central camera on the right side. - /camera0/camera_info – Intrinsic and distortion information of left camera. - /camera0/projection_matrix – Extrinsic matrix of left camera from lidar. - /camera2/camera_info – Intrinsic and distortion information of central camera. - /camera2/projection_matrix – Extrinsic matrix of central camera from lidar. - /camera5/camera_info – Intrinsic and distortion information of right camera. - /camera5/projection_matrix – Extrinsic matrix of right camera from lidar. - /novatel/oem7/bestpos – Latitude, longitude, and elevation information from NovAtel GNSS-INS system. - /points_raw – VLP-32 lidar point cloud. - /tf – Vehicle base frame. The data are organized into a data description file and one or more ROS .bag files, dependent on original file size. The data description file provides information about the data collection date, location, and detailed mapping, while the .bag file(s) contain the actual data. Please note that for the purpose of securing personally identifiable information, all license plates and faces included in this publication have been intentionally blurred during real-time processing. ![ashland avenue image](ashland-avenue.png)

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Immobilizing Pertechnetate in Ettringite via Sulfate Substitution

Until recently, a nuclear waste form did not exist for the immobilization and long-term storage of the anionic form of radionuclide technetium-99 (99Tc), pertechnetate (TcO 4 - ). Across international nuclear waste sites, the inability to capture TcO 4 - poses a threat to the local environment due to the anion’s long half-life and environmental mobility under environmentally oxic conditions. To combat this challenge, most waste forms would capture 99Tc using materials that reduce TcO 4 - to Tc(IV) species, e.g. 99Tc oxides or 99Tc sulfides. However, this is a short-lived solution unless reducing capacities can be regenerated to last over the long life expectancy of some nuclear waste forms (~10,000 years). In light of recent experimental observations gained from the development of cementitious waste forms and unconfirmed hypotheses from the literature, this work explores how ettringite, a common mineral formed in cementitious materials with demonstrated success in incorporating oxyanions, may be used to immobilize TcO 4 - directly and over the life-time of the waste form. Using batch precipitation experiments, solid phase characterization techniques, and ab initio molecular dynamics simulations, we demonstrate herein successful incorporation of TcO 4 - into ettringite via substitution for SO 4 2- within the ettringite crystal structure. Here, these results are first of their kind and confirm the hypothesis that ettringite acts as an immobilizing mineral within cementitious waste forms for the highly mobile TcO 4 - oxyanion, enhancing the overall performance of these waste forms over time.

36 MATERIALS SCIENCE↗

Viral Infection of Subsurface Microorganisms and Metal/Radionuclide Transport (Final Technical Report)

Microbially mediated metabolisms have been identified as a significant factor either directly or indirectly impacting the fate and transport of heavy metal/radionuclide contaminants. To date microorganisms have been isolated from contaminated environments. Examination of annotated finished genome sequences of many of these subsurface isolates from DOE sites, revealed evidence of prior viral infection. To date the role that viruses play influencing microbial mortality and the resulting community structure which directly influences biogeochemical cycling in soils and sedimentary environments remains poorly understood. The objective of this exploratory study was to investigate the role of viral infection of subsurface bacteria and the formation of contaminant-bearing viral particles. This objective was approached by examining the following working hypotheses: (i) subsurface microorganisms are susceptible to viral infections by the indigenous subsurface viral community, and (ii) viral surfaces will adsorb heavy metals and radionuclides. Our results have addressed basic research needed to accomplish the BER Long Term Measure to provide sufficient scientific understanding such that DOE sites would be able to incorporate coupled physical, chemical and biological processes into decision making for environmental remediation or natural attenuation and long-term stewardship by establishing viral-microbial relationships on the subsequent fate and transport of heavy metals and radionuclides. Here we demonstrated that viruses play a significant role in microbial mortality and community structure in terrestrial subsurface sedimentary systems. The production of viral-like particles within subsurface sediments in response to biostimulation with dissolved organic carbon and a terminal electron acceptor resulted in the production of viral-like particles. Organic carbon alone did not result in significant viral production and required the addition of a terminal electron acceptor (nitrate), indicating that nutrients are not limiting viral production, but rather substrates that can be converted into energy for host metabolism. Our results also revealed that cell abundance was not correlated to the mineralization of organic carbon, but rather viruses were positively correlated with carbon mineralization. This is a result of viral-mediated cell lysis and demonstrates that viruses are sensitive indicators of microbial activity. Viruses as an indicator of microbial activity was not unique to batch culture studies as results obtained from an in situ field experiment conducted at the DOE Old Rifle Field site. This study revealed that viral abundance increased in response to the injection of oxygenated groundwater and influx of dissolved organic carbon whereas cell abundance changes were minimal. However, the extent to which viral-mediated cell lysis alters organic matter pools subsequently influencing microbial community structure and biogeochemical function remains a critical question in subsurface biogeochemical cycling.

54 ENVIRONMENTAL SCIENCES↗

Fluid Induced Elemental and Mineralogy Alterations of Caney Shale

ABSTRACT: Studies were conducted on cores and rock cuttings recovered from two wells drilled in Caney shale in the Southern Oklahoma. Mineralogical compositions of these samples were obtained by X-Ray Diffraction (XRD) measurements using two methods of sample preparation: conventional powder (by crushing and grinding of rock fragments) and spray-drying of micronized rock powder method. Microstructure and microanalysis were acquired by Scanning Electron Microscopy/Energy Dispersive Spectroscopy (SEM/EDS). Batch experiments were then conducted using selected rock samples and fracturing fluid whilst deionized water was used as control sample for fluid/rock interaction. These were conducted at 95°C and ambient pressure for various time periods to assess the geochemical reactivity of the Caney shale. The rock samples were subsequently recovered from fluid, dried and analysis repeated using identical XRD and SEM/EDS measurements, following the same conditions. Preliminary experimental results show rock mineralogical compositions are predominantly quartz with relatively high clay content. The clay minerals are mainly illite. Carbonate content is less than 10% by weight for most samples, with other non-clay minerals pyrite, albite, dolomite, and some apatite. In general, sprayed samples showed more intense peaks and less full width at half maxima (FWHM) relative to conventional rock-powder samples. Post-experimental mineralogical changes were observed in samples with clay portions breaking down to amorphous entities. As expected, dissolution of carbonates (calcite and dolomite) was observed and newly detected dissolution of biogenic micro quartz resulted in formation of amorphous silica. 1.0 INTRODUCTION Formation of sedimentary rocks involves processes where rock sediments are emplaced with fluids starting interactions that persist over long periods. During the lithification process, sediments and fluids react and attain equilibrium state. This equilibrium is disturbed during drilling, completion, hydraulic fracturing and other operations that involve the introduction of engineered fluids into the subsurface. To return to equilibrium, dissolution and precipitation of minerals may occur. These reactions have implications on the petrophysical properties of the reservoir. Whiles dissolution and precipitation of minerals can enhance porosity and permeability, the reverse can also be true. For example, when acidic fluids are introduced into formations with high carbonate contents, carbonate minerals dissolve into solution thus increasing the porosity and permeability of the formation. In contrast, when alkaline fluids with pH above 11 are introduced into an illite-rich shale formation, the rock-fluid interaction leads to de-flocculation of illite platelets causing substantial increase in clay fines migration, consequently significant reduction in permeability (Salles et al., 2008).

Awejori, G.↗

Simulation of the Quality Criterion of a Mixture in a Drum-Belt Apparatus

A method is proposed for calculating the inhomogeneity coefficient in the workspace of a drum-belt mixer of bulk components with brush elements in a three-stage batch mixing method with non-uniform proportioning. The method is based on a stochastic model of the motion of rarefied particle flows following interaction with flexible elements fixed along a helical line on the surface of the mixer drums. The principal coefficients affecting the quality of a bulk mixture are analyzed in the form of combined structural and regime complexes of parameters of the mixer and the characteristics of the physical and mechanical state of the mixed media are analyzed. The results obtained can be used to develop an engineering technique for calculating the parameters of a new drum-belt mixer of friable components.

42 ENGINEERING↗

Purification of Zirconium Tetrachloride from UNF Cladding

The overarching objective of this project was to design and demonstrate (laboratory scale) a sublimation-based purification protocol to obtain pure zirconium chloride (ZrCl 4 ) from impure feeds derived from the direct chlorination of Zircaloy cladding materials. To achieve this objective the following goals were identified. (1) Design, construct and test an apparatus capable of subliming and purifying ZrCl 4 at room pressure and temperatures between 600 and 700K (sublimation point of ZrCl 4 606 K). (2) Investigate reactions that may be used to chemically alter the makeup of the impure ZrCl 4 feed materials to enhance their removal from ZrCl 4 in the sublimation-purification process. (3) Computationally model the reactions of metal chlorides in the gas phase under sublimation conditions (1 atm, 600 K) to determine if oligomers are formed and, if formed, how they would influence sublimation-based purification strategies. All experimental investigations performed as part of this project used stable (non-radioactive) compounds and materials as surrogates for the impure ZrCl 4 feedstocks that would be derived from the direct chlorination of Zircaloy claddings from spent nuclear fuel rods. No radiologically active materials were used at any time in this project. The impure ZrCl 4 feedstocks used in this study were derived from the direct chlorination of virgin Zircaloy claddings (Zirc-2, -4 and high Nb). The main goals of the project have been achieved during the three year period of this NEUP sponsored project. The impurities of greatest concern in the feedstocks were identified as the chloride salts of the alloying metals originally found in Zircaloy (Fe, Nb) and radiological contaminants (Cs, Sr, and Sb). A series of prototype sublimation apparatuses and heating arrangements were designed, constructed and tested. A general batch-sublimator design was identified and a 1.0 kg batch sublimator/oven system was fabricated from glass. Purification protocols developed on small scale runs were found to scale to 1.0 kg batches without problem. Purification factor ranges (PFs: wt% final / wt% initial ) for the impurity chlorides identified above have been measured: Fe (40 – 500); Nb (10 – 70); Cs (520 – 5000); Sr (250 – 1900); Sb (220 – 2300). Removal of iron is sensitive to the partial pressure of hydrogen (in nitrogen) flowing through the system. Lower PFs are obtained when the hydrogen partial pressure is lower. Lower flows are required to raise the iron PF. Removal of niobium is very sensitive to the endpoint determination of the forerun. When judged properly (color change yellow to white in sublimate) reasonable PFs (500) can be achieved. However, as discussed in the conclusions section, endpoint determination can be difficult and significantly lower PFs may be obtained when the endpoint is not correctly identified. Several methods of obtaining quantitative cesium, strontium and antimony PFs were investigated, the best being ICP-MS. The results reported here reflect very limited access to and ICP-MS instrument during the course of this project. It should be noted that, while significantly reduced amounts of antimony are observed in the product, antimony is also found in the exhaust trap after the condenser. Quantum chemical computational modeling studies of the reactions of metal chlorides in the gas phase provided important information about a chemical transport mechanism that could defeat sublimation-based purification strategies. Many metal chlorides are known to oligomerize in the gas phase to reduce their coordinative unsaturation. Dimerization of ZrCl 4 with iron or niobium chlorides would provide a mechanism by which both metal impurities could be carried over with the product during sublimation of the bulk material. Computational modeling conclusively showed that under sublimation conditions in the gas phase, dimerization reactions are not favored thermodynamically due to a significant entropic penalty for the reaction. Therefore, consistent with experimental observations, sublimation-based purification strategies remain viable. The experimental part of the report concludes with a short discussion of the issues that still remain in developing a technologically relevant Zircaloy recycling strategy. The final section of the report is a summary of the quantum chemical investigation of the reactions of metal chlorides in the gas phase under sublimation conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Technetium Getters to Improve Cast Stone Performance

The cementitious material known as Cast Stone has been selected as the preferred waste form for solidification of aqueous secondary liquid effluents from the Hanford Tank Waste Treatment and Immobilization Plant (WTP) process condensates and low-activity waste (LAW) melter off-gas caustic scrubber effluents. Cast Stone is also being evaluated as a supplemental immobilization technology to provide the necessary LAW treatment capacity to complete the Hanford tank waste cleanup mission in a timely and cost effective manner. Two radionuclides of particular concern in these waste streams are technetium-99 (99Tc) and iodine-129 (129I). These radioactive tank waste components contribute the most to the environmental impacts associated with the cleanup of the Hanford site. A recent environmental assessment of Cast Stone performance, which assumes a diffusion controlled release of contaminants from the waste form, calculates groundwater in excess of the allowable maximum permissible concentrations for both contaminants. There is, therefore, a need and an opportunity to improve the retention of both 99Tc and 129I in Cast Stone. One method to improve the performance of Cast Stone is through the addition of “getters” that selectively sequester Tc and I, therefore reducing their diffusion out of Cast Stone. In this paper, we present results of Tc and I removal from solution with various getters with batch sorption experiments conducted in deionized water (DIW) and a highly caustic 7.8 M Na Ave LAW simulant. In general, the data show that the selected getters are effective in DIW but their performance is comprised when experiments are performed with the 7.8 M Na Ave LAW simulant. Reasons for the mitigated performance in the LAW simulant may be due to competition with Cr present in the 7.8 M Na Ave LAW simulant and to a pH effect.

Cast Stone↗

Striped Data Analysis Framework

Traditionally, High Energy data analysis is based on the model where data are stored in files and analyzed by running multiple analysis processes, each reading one or more of the data files. This process involves repeated data reduction step, which produces smaller files, which is time consuming and leads to data duplication. We propose an alternative approach to data storage and analysis, based on the Big Data technologies. The idea is to store each element of data once and only once in a distributed scalable database and analyze data by reading only "interesting" pieces of data from the database. To make this approach possible, we developed columnar Striped Data Representation Format as the basis of the framework. Traditional columnar approach allows for efficient analysis of complex data structures. While keeping all the benefits of columnar data representation, striped mechanism goes further by enabling efficient parallelization of computations and flexible dist ribution of data analysis. The framework includes scalable and elastic data storage, compute and user analysis backend components. The framework uses off-the shelf web services and data caching technologies as the compute/data co-location mechanism. Flexible architecture allows the framework run in the cloud using container technologies. The framework offers Python/Jupyter as the user analysis backend platform, but can also run in command line or batch mode. In the article, we will present the results of the FNAL-LDRD-2016-032 FNAL LDRD project, the design, implementation, features and performance characteristics of the Striped Data Analysis Framework.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Raw_data_Batch_I: Lisle to Waterfall Glen

Date of collection: May 11, 2023 Location: DuPage County, IL This dataset contains lidar and vision data collected between Lisle, IL, and the Waterfall Glen parking lot. The vehicle started near Cass School District 63, headed east along IL 34. The vehicle then turned south along IL 83 until Interstate 55. Finally, the vehicle turned southwest along I 55 until Exit 273A and headed toward the Waterfall Glen parking lot. The data contains the following Robot Operating System (ROS) topics: - /Central_Camera_blurred – Image flow from coaxial camera heading, vehicle front. - /Left_Camera_blurred – Image flow from left camera, 60° from central camera on the left side. - /Right_Camera_blurred – Image flow from right camera, 60° from central camera on the right side. - /camera0/camera_info – Intrinsic and distortion information of left camera. - /camera0/projection_matrix – Extrinsic matrix of left camera from lidar. - /camera2/camera_info – Intrinsic and distortion information of central camera. - /camera2/projection_matrix – Extrinsic matrix of central camera from lidar. - /camera5/camera_info – Intrinsic and distortion information of right camera. - /camera5/projection_matrix – Extrinsic matrix of right camera from lidar. - /novatel/oem7/bestpos – Latitude, longitude, and elevation information from NovAtel GNSS-INS system. - /points_raw – VLP-32 lidar point cloud. - /tf – Vehicle base frame. The data are organized into a data description file and one or more ROS .bag files, dependent on original file size. The data description file provides information about the data collection date, location, and detailed mapping, while the .bag file(s) contain the actual data. Please note that for the purpose of securing personally identifiable information, all license plates and faces included in this publication have been intentionally blurred during real-time processing. ![lisle waterfall image](lisle-waterfall.png)

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Bayesian batch optimization for molybdenum versus tungsten inertial confinement fusion double shell target design

Access to reliable, clean energy sources is a major concern for national security. Much research is focused on the “grand challenge” of producing energy via controlled fusion reactions in a laboratory setting. For fusion experiments, specifically inertial confinement fusion (ICF), to produce sufficient energy, the fusion reactions in the ICF fuel need to become self-sustaining and burn deuterium-tritium (DT) fuel efficiently. The recent record-breaking NIF ignition shot was able to achieve this goal as well as produce more energy than used to drive the experiment. This achievement brings self-sustaining fusion-based power systems closer than ever before, capable of providing humans with access to secure, renewable energy. In order to further progress toward the actualization of such power systems, more ICF experiments need to be conducted at large laser facilities such as the United States's National Ignition Facility (NIF) or France's Laser Mega-Joule. The high cost per shot and limited number of shots that are possible per year make it prohibitive to perform large numbers of experiments. As such, experimental design relies heavily on complex predictive physics simulations for high-fidelity “preshot” analysis. These multidimensional, multi-physics, high-fidelity simulations have to account for a variety of input parameters as well as modeling the extreme conditions (pressures and densities) present at ignition. Such simulations (especially in 3D) can become computationally prohibitive to turn around for each ICF experiment. In this work, we explore using Bayesian optimization with Gaussian processes (GPs) to find optimal designs for ICF double shell targets, while keeping computational costs to manageable levels. These double shell targets have an inner shell that grades from beryllium on the outer surface to the higher Z material molybdenum, as opposed to the nominally used tungsten, on the inside in order to trade off between the high performance associated with high density inner shells and capsule stability. We describe our results for “capsule-only” xRAGE simulations to study the physics between different capsule designs, inner shell materials, and potential for future experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Raw_data_Batch_I: Lakeshore Drive

Date of collection: May 18, 2023 Location: Lakeshore Drive, Chicago, IL Content: “North to South” “South to North” This data set contains lidar and vision data collected along Lakeshore Drive. The “South to North” folder starts from the intersection of Lakeshore Drive and 31st Street and ends at Hollywood Towers Chicago. The “North to South” folder starts from the intersection of Lakeshore Drive and Sheridan Avenue and ends at the 31st Street intersection. The data contains the following Robot Operating System (ROS) topics: - /Central_Camera_blurred – Image flow from coaxial camera heading, vehicle front. - /Left_Camera_blurred – Image flow from left camera, 60° from central camera on the left side. - /Right_Camera_blurred – Image flow from right camera, 60° from central camera on the right side. - /camera0/camera_info – Intrinsic and distortion information of left camera. - /camera0/projection_matrix – Extrinsic matrix of left camera from lidar. - /camera2/camera_info – Intrinsic and distortion information of central camera. - /camera2/projection_matrix – Extrinsic matrix of central camera from lidar. - /camera5/camera_info – Intrinsic and distortion information of right camera. - /camera5/projection_matrix – Extrinsic matrix of right camera from lidar. - /novatel/oem7/bestpos – Latitude, longitude, and elevation information from NovAtel GNSS-INS system. - /points_raw – VLP-32 lidar point cloud. - /tf – Vehicle base frame. The data are organized into a data description file and one or more ROS .bag files, dependent on original file size. The data description file provides information about the data collection date, location, and detailed mapping, while the .bag file(s) contain the actual data. Please note that for the purpose of securing personally identifiable information, all license plates and faces included in this publication have been intentionally blurred during real-time processing. ![lakeshore drive image](lakeshore-drive.png)

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Modified Isotherm Modeling to Predict Cs Exchange with Crystalline Silicotitanate in Tank Waste Simulants

The U.S. Department of Energy is working to expedite processing of Hanford tank waste supernate at the Hanford Waste Treatment and Immobilization Plant. To support this goal, Washington River Protection Solutions is designing a Tank Side Cesium Removal (TSCR) system for suspended solids and cesium (Cs/ 137 Cs) removal from Hanford tank waste supernate. The ion exchange media selected for Cs removal at TSCR is crystalline silicotitanate (CST) that is manufactured in a nearly spherical form by Honeywell UOP LLC (UOP; Des Plaines, IL) as product IONSIV® R9140-B (Na form). The Zheng Anthony Miller (ZAM) isotherm model (Zheng et al. 1997) is a multicomponent ion exchange model used to predict the exchange of Group I metals onto CST. The ZAM isotherm has historically been used to predict Cs distribution values from Hanford and Savannah River Site (SRS) tank waste simulants. Figure S.1 summarizes model predictions from the ZAM isotherm that indicate poor prediction of Cs distribution values for simple and complex simulants with the engineered form of CST, IONSIV® R9140-B, and IONSIV® R9120-B where the solid line indicates a perfect fit by the model. The dotted lines indicate ±20% error. Batch contact testing with Hanford tank waste complex and simple simulants was used in conjunction with SRS simulants to experimentally determine Cs distribution values using a modification to the original isotherm model. The experimentally determined maximum Cs capacity for IONSIV® R9140-B CST in both the simple and complex matrices was found to be 0.53±0.3 mmoles Cs/g of CST. This value is not drastically different from the maximum Cs capacity of 0.58 mmoles Cs/g TAM-5 reported by Zheng et al. (1997). However, it is important to note that TAM-5 (commercially IONSIV® IE-910) is a powder. Hamm et al. (2002) determined that a dilution factor was needed to account for the Zr(OH)2 binder in the engineered form of CST. Hamm et al. determined that a dilution factor of 0.68 was appropriate to account for binder contribution and correct overprediction of Cs exchange on the engineered form of CST in ZAM calculations. This reduced the total capacity from 0.58 mmol/g with TAM-5 to 0.39 mmol/g for the engineered form of CST (Hamm et al. 2002). Despite substituting the experimentally determined maximum Cs capacity of 0.55 mmoles Cs/g for the literature-reported capacity of 0.39 mmoles Cs/g, it was determined that additional modifications to the model’s equilibrium rate constants were necessary in refining the isotherm model. The modified model overpredicted K+ uptake by the CST when compared to digested CST results described by Campbell et al. (2019). The modified model was further revised to omit three of the five K+ exchange equilibrium reactions described by ZAM to reduce the additional K+ loading seen by the model. Figure S.2 summarizes the revised model isotherm predictions plotted against measured Kd values.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

High-Temperature Creep Behavior of Thin-Walled FeCrAl Alloy Tubes

This report summarizes measured creep properties for FeCrAl alloy C26M measured using subsized specimens machined from prototypic thin-walled tubes. A representative tube fabricated in a previous large batch production effort was machined into dual-gauge axial specimens using electrical-discharge machining. Creep tests, comprising strain-rate jump tests (SRJ), jump stress (JS) and constant-stress (CS) tests, were conducted at temperatures ranging from 600-900ºC to determine creep mechanisms (elucidated from stress exponents) and activation energies to compare with prior data available in the literature at temperatures up to 650ºC. It was found that the results from the SRJ tests indicated that the highest stress exponent of 5.8 occurred at 600ºC, which decreased to the lowest stress exponent of 2.5 at 700ºC. At higher temperatures, the stress exponents increased slightly to a range of 2.9 to 4.3 between 750ºC and 900ºC. The high stress exponent value of 5.8 suggested dislocation glide creep mechanisms dominated creep deformation at 600ºC since high stress values were measured. The low stress exponent of 2.5 at 700ºC suggested diffusional creep mechanisms start to occur that aid in dislocation cross-slip and climb mechanisms. The slightly higher stress exponents of 2.9 to 3.9 may suggest different contributions of creep deformation mechanisms based on diffusional processes associated with Nabarro-Herring and Coble creep and dislocation creep that involve thermally activated cross-slip and climb mechanisms. These deformation mechanisms could have also been affected by the development of recovery and/or recrystallization processes in the microstructure of the C26M2 specimens. From the SJ and single CS tests, two sets of creep activation energies were calculated. The steady state creep values obtained from the SJ tests showed several abnormalities especially with the data at 850ºC. The comparison of the creep activation energies between the data from the SJ and CS tests showed higher creep rates for the SJ tests than the CS tests, indicating microstructure softening occurred in the C26M2 specimens during the SJ tests that led to the higher creep rates at stresses above the initial stress of 10 MPa. For the CS tests, the results showed steady increases in MCR with increasing temperature at each stress. The best linear fit to the MCR values at each stress was with data obtained at 800ºC, 850ºC and 900ºC. The lowest Q c value of 130.8 KJ/mole was observed with the highest stress of 25 MPa. As stress was lowered, the Q c values increased continuously to the highest value of 188.2 KJ/mole at 10 MPa. This trend suggests that the dominant creep mechanism is diffusional based dislocation climb since the decreasing activation energies with increasing stress promotes easier dislocation climb around obstacles. The comparison between the SJ and CS tests indicates that the best type of creep test performed on FeCrAl alloys such as C26M2 is the single CS test.

36 MATERIALS SCIENCE↗

Automatic Synthesis of Multimodal Polymers

An automatic molecular weight controller is used in semi-batch reactions to produce final polymers that contain distinct subpopulations with different molecular weight distributions (MWD). While blending polymers with different MWD is frequently used to make multimodal polymer products, a method is introduced here allowing the multimodal product to be made in successive, automatically controlled stages in the same reactor. The method is demonstrated using free radical polymerization of acrylamide to produce widely separated multimodal MWD. Automatic Continuous Online Monitoring of Polymerization reactions with a Control Interface (ACOMP/CI) was used. Weight average molecular weight (M w ) in the ACOMP/CI was continuously measured with multi-angle light scattering and ultra-violet absorption. The controller used two principles: both polymerization rate and instantaneous molecular weight are proportional to monomer concentration. By controlling monomer flow rate into the reactor, the controller produced a targeted amount of polymer with a desired first M w and then automatically introduced chain transfer agent (CTA) into the reactor to produce a second population of polymers with much lower M w . Subsequently, reactions were performed to produce trimodal populations. Finally, this approach is kindred to multi-stage synthesis of polymers where distinctly different processes are carried out in succeeding stages to produce polymers with highly specific properties.

42 ENGINEERING↗

Selective separation of Sr by potassium titanates from solution of nitrate - 15248

The radioactive waste treatment is planned in LWTF (Low-level radioactive Waste Treatment Facility, JAEA) for the low-level liquid wastes generated from Tokai-reprocessing facility [1]. The target liquid wastes mainly consist of highly concentrated sodium nitrate (4.7 M NaNO{sub 3}) containing low level radioactive {sup 137}Cs and {sup 90}Sr, while the conventional adsorbent (Titanic acid-PAN) has some problems in the adsorption performance and irradiation resistance. In this study, the adsorption properties of Sr{sup 2+} ions, leaching properties of Sr{sup 2+} and irradiation properties were clarified by using the novel adsorbent of potassium titanates (KT-1). Relatively large uptake percentage (99%) and maximum uptake capacity (0.37 mmol/g) were obtained for the KT-1 compared to that of Titanic acid-PAN. As for the breakthrough properties, KT-1 had the smoother breakthrough carve and larger 5% breakthrough capacity compared to Titanic acid-PAN. From the results of batch and column experiments, KT-1 was effective for the uptake of Sr{sup 2+} ions in the presence of highly concentrated Na{sup +} ions. The leached percentages of Sr{sup 2+} ions form calcined products of Sr-KT-1 in pure water and 0.1 M NaOH were less than the detection limit of ICP-AES, and those in 0.1 M HCl tended to markedly decrease with calcining temperature; the formation of SrTiO{sub 3} phase above 800 deg. deg. C was effective for the lowering of leachability. The irradiation stability of the adsorbent was examined by instrumental analyses and the evaluation for the uptake percentage of Sr{sup 2+} ions by batch method. The growth of surface crystal was observed by SEM, but no significant change in X-ray diffraction peak was observed, and Sr{sup 2+} uptake (%) was almost constant. The novel adsorbent of KT-1 had excellent characteristics for Sr selectivity, uptake capacity, leachability and irradiation resistance. KT-1 is thus effective for the treatment and disposal in LWTF. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Impact of Concurrent Solubilization and Fines Migration on Fracture Aperture Growth in Shales during Acidized Brine Injection

Acidic hydraulic fracturing fluid chemically and physically alters shale rock fabric during injection and shut-in, creating a “reaction-altered zone” along the fracture faces. To better characterize the variable thickness and composition of this reaction-altered zone under advective flow, we take a coupled experimental and modeling approach. A fluidic cell, with six fiducial markers, is first fabricated to keep the rock sample in place during the core floods and to allow image alignment of acquired images. Then, we conduct a series of reactive core floods in a clay-rich siliceous Wolfcamp shale sample with 10 wt % carbonate, using a synthetic fracturing fluid under no confining stress and at room temperature. High-resolution computed tomography (CT) scans are periodically conducted to observe the spatial alteration of the fracture network. We then perform scanning electron microscopy (SEM-EDS) on the two orthogonal surfaces (fracture surface and freshly cut profile face) to generate high-resolution elemental maps that show the change in mineralogy, both with distance along a given flow path along a fracture surface and with depth from the fracture surface into the shale matrix. These results are contrasted against a two-dimensional (2D) advection-diffusion reaction model developed previously for batch reactions between shale and synthetic fracturing fluids. The model simulates the geochemical interaction occurring at the fracture/matrix interface and penetrating into the shale matrix during the reactive core flood. Both model and experimental results show that the acidic brine is neutralized during the core flood, corresponding to an increase in fracture aperture as a function of fluid volume injected with the greatest change near the inlet. SEM-EDS scans reveal significant dissolution of carbonates on the fracture surface without pyrite oxidation. The reactive transport model indicates that carbonate depletion into the shale interior should be observable, yet SEM-EDS shows no discernible loss of carbonate in the orthogonal profile face. The combination of these observations suggests an additional fracture evolution mechanism in the reactive system, i.e., fines migration. We show that fines migration enhances the access of fracturing fluid to the matrix resulting in a more pronounced fracture widening. Finally, we conclude that coupled mineral dissolution and fines migration govern fracture aperture growth during acidized brine injection. In this work, we effectively show the underlying risk of relying solely on models that do not include an important (transport) process that can alter the system significantly and propose a combined chemomechanical mechanism for fracture evolution appropriate for this shale mineralogy.

58 GEOSCIENCES↗

Indonesian Highly Enriched Uranium-Bearing Waste Elimination - 17393

The Department of Energy's National Nuclear Security Administration (NNSA) and the Y-12 National Security Complex (Y-12) have been working with PT Industri Nuklir Indonesia (PT Inuki), an Indonesian medical isotope producer, since 2014 to disposition all highly enriched uranium (HEU) stored at the government-owned Research Center for Science and Technology (PUSPIPTEK) near Serpong, Indonesia. To eliminate the 1.5 kilograms of liquid HEU at the facility, Y-12 proposed a method to down-blend the leftover process solutions with a depleted uranium solution made on-site to render low-enriched uranium (LEU). This method is essentially irreversible since the uranium enrichment is degraded using a molecular level of intimate mixing in aqueous solution. This cooperation was tied to a presidential commitment made at the 2016 Nuclear Security Summit to down-blend all remaining HEU in Indonesia by September 2016. While all unirradiated HEU was down-blended to LEU in March 2016, the campaign to down-blend the 1.4 kilograms of irradiated HEU began in late July 2016 and was completed in August, making Indonesia and all of Southeast Asia free of HEU. As part of this cooperation, Y-12 and NNSA also proposed a subsequent disposition option for the LEU solution whereby the irradiated and unirradiated solutions will be chemically manipulated to prepare a dry LEU oxide suitable for interim storage and yield a uranium-free liquid stream that can be discarded as radioactive waste. In the fall of 2016, Y-12 and NNSA plan to begin developing the LEU solution disposition methodology with the Indonesian facility using small-scale batch-wise methods within existing hot cells, involving straightforward precipitation, ion exchange, decantation, and calcination methods. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Extending Magnetic Core Shell Nanoparticle Extraction Technology to Cesium and Antimony Removal from Geothermal Brines in New Zealand

Our industrial client (Geo40) has developed and deployed a process to remove silica from geothermal fluids and produce a high-margin specialty colloidal silica product comparable to those of market leaders. Geo40 now wishes to explore opportunities to extend their mineral extraction operations to other elements that are present in these brines. Geo40 has identified cesium (Cs) that is present in Ohaaki brines (pH ~8–8.5) at parts per million levels and could be sold to customers if it could be produced at an attractive price. With support from the Department of Energy’s (DOE’s) Geothermal Technologies Office, a simple and highly cost-effective magnetic nanofluid method for extraction of rare earth elements (REEs) from geothermal brine solutions has been developed and demonstrated at the laboratory bench scale at Pacific Northwest National Laboratory (PNNL). Core shell sorbent particles are produced using an iron oxide core particle, which is used to anchor and grow a surrounding adsorbent shell functionalized with a chelating ligand that selectively binds REEs. We extended PNNL’s work by exploring new sorbent shells that are highly selective for Cs. Uptake of Cs was measured as a function of exposure time by analyzing solution samples extracted from batch sorption tests.

15 GEOTHERMAL ENERGY↗