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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5

Bayesian learning with Gaussian processes for low-dimensional representations of time-dependent nonlinear systems

This work presents a data-driven method for learning low-dimensional time-dependent physics-based surrogate models whose predictions are endowed with uncertainty estimates. We use the operator inference approach to model reduction that poses the problem of learning low-dimensional model terms as a regression of state space data and corresponding time derivatives by minimizing the residual of reduced system equations. Standard operator inference models perform well with accurate training data that are dense in time, but producing stable and accurate models when the state data are noisy and/or sparse in time remains a challenge. Another challenge is the lack of uncertainty estimation for the predictions from the operator inference models. Our approach addresses these challenges by incorporating Gaussian process surrogates into the operator inference framework to (1) probabilistically describe uncertainties in the state predictions and (2) procure analytical time derivative estimates with quantified uncertainties. The formulation leads to a generalized least-squares regression and, ultimately, reduced-order models that are described probabilistically with a closed-form expression for the posterior distribution of the operators. The resulting probabilistic surrogate model propagates uncertainties from the observed state data to reduced-order predictions. Furthermore, we demonstrate the method is effective for constructing low-dimensional models of two nonlinear partial differential equations representing a compressible flow and a nonlinear diffusion–reaction process, as well as for estimating the parameters of a low-dimensional system of nonlinear ordinary differential equations representing compartmental models in epidemiology.

Data-driven model reduction↗

Stabilization/Solidification of Tritiated Water - 20135

Tritiated water was stabilized/solidified by using calcium oxide and a polymer. First, tritiated water was changed into the powder form of calcium hydroxide by addition of tritiated water into calcium oxide. Then the produced calcium hydroxide was solidified in waste form by using a polymer binder. The specimens of waste form prepared by surrogate calcium hydroxide were subjected to compressive strength testing and water immersion testing. In addition, the specimens of waste form prepared by tritiated calcium hydroxide were subjected to leach testing. The mean compressive strength of the specimens containing 40 wt % of the surrogate calcium hydroxide was about 98.5 MPa (14,300 psi). After water immersion testing, there was no distinct change in the appearance of the specimens. The mean compressive strength of the specimens after water immersion was 79.1 MPa (11,470 psi). The mean diffusion coefficient of tritium for the specimens containing 40 wt% of tritiated calcium hydroxide was 5.4 x 10-10 cm{sup 2}/s. These findings indicate that the waste form has enough mechanical integrity and durability for final disposal and releases tritium very slowly. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Comparisons of Mixing Efficiency for the Strut Fuel Injector Obtained from Large-Eddy and Reynolds-Averaged Simulations, and Experiments

Mixing efficiency is obtained for a strut fuel injector at hypervelocity flow conditions by using large-eddy simulations (LES), Reynolds-averaged simulations (RAS), and experiments. The injector and flow conditions have been previously investigated by using RAS and experiments as a part of the Enhanced Injection and Mixing Project (EIMP) at the NASA Langley Research Center (LaRC). Because the fidelity of LES is a strong function of the grid, the mixing efficiency is obtained on two grids, the coarser of which is a factor of two coarser in each of the three dimensions with respect to the fine grid. The RAS uses the two-equation linear eddy viscosity and diffusivity modeling of Menter. In RAS, the species diffusivity model exhibits a strong dependence on the turbulent Schmidt number, which is often adjusted until some metric of engineering interest, such as the mixing efficiency, matches the experimental data. In the absence of experimental data, scale-resolving simulations, such as LES, have been proposed as surrogates for experiments that could provide the data needed to “calibrate” the turbulent Schmidt number in the RAS models. This approach is followed because LES requires significantly more computational resources (CPU, data storage, and time) than RAS, making it prohibitive for use in many engineering applications and specifically for parameter exploration or optimization. Here we examine the mixing efficiency obtained from several RAS with different values of the turbulent Schmidt number, and compare the results with those obtained from the LES and experiments. In addition, the least squares fitting approach was used to demonstrate how to obtain an estimate for the turbulent Schmidt number from LES analytically. These estimates were then used together with prior knowledge about RAS model sensitivity to select a turbulence model that was expected to best match the LES data.

LES↗

Comparisons of Mixing Efficiency for the Strut Fuel Injector Obtained from Large-Eddy and Reynolds-Averaged Simulations, and Experiments

Mixing efficiency is obtained for a strut fuel injector at hypervelocity flow conditions by using large-eddy simulations (LES), Reynolds-averaged simulations (RAS), and experiments. The injector and flow conditions have been previously investigated by using RAS and experiments as a part of the Enhanced Injection and Mixing Project (EIMP) at the NASA Langley Research Center (LaRC). Because the fidelity of LES is a strong function of the grid, the mixing efficiency is obtained on two grids, the coarser of which is a factor of two coarser in each of the three dimensions with respect to the fine grid. The RAS uses the two-equation linear eddy viscosity and diffusivity modeling of Menter. In RAS, the species diffusivity model exhibits a strong dependence on the turbulent Schmidt number, which is often adjusted until some metric of engineering interest, such as the mixing efficiency, matches the experimental data. In the absence of experimental data, scale-resolving simulations, such as LES, have been proposed as surrogates for experiments that could provide the data needed to “calibrate” the turbulent Schmidt number in the RAS models. This approach is followed because LES requires significantly more computational resources (CPU, data storage, and time) than RAS, making it prohibitive for use in many engineering applications and specifically for parameter exploration or optimization. Here we examine the mixing efficiency obtained from several RAS with different values of the turbulent Schmidt number, and compare the results with those obtained from the LES and experiments. In addition, the least squares fitting approach was used to demonstrate how to obtain an estimate for the turbulent Schmidt number from LES analytically. These estimates were then used together with prior knowledge about RAS model sensitivity to select a turbulence model that was expected to best match the LES data.

LES↗

Kinetics and Mechanism of Tetravalent Cerium Extraction by Di-2-Ethylhexyl Isobutyramide (DEHiBA)

DEHiBA is a fully-incinerable, CHON extractant with a high selectivity for hexavalent actinides. However, as a recently-developed ligand, much remains unknown about its physical and chemical properties, including its extraction and phase disengagement rates. Here, we present data on the phase transfer kinetics of Ce(IV) extraction and stripping by both DEHiBA and TBP collected using microfluidic devices. Ce(IV) was selected as a surrogate for Pu(IV) and Np(IV) in the initial tests of the microfluidics system prior to testing with the actinides. Pseudo first-order reaction rate constants are determined for both systems, and the corresponding Damköhler numbers (Da) are calculated to establish whether the extraction and stripping processes are kinetically or diffusion controlled. The stoichiometry of the extracted Ce(IV)-DEHiBA complex is determined, and the phase disengagement properties under extraction conditions are assessed using the dimensionless dispersion number. A possible explanation for the favorable extraction of Ce(IV) by DEHiBA, which is known to poorly extract many tetravalent cations, is presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Taylor approximation variance reduction for approximation errors in PDE-constrained Bayesian inverse problems

In numerous applications, surrogate models are used as a replacement for accurate parameter-to-observable mappings when solving large-scale inverse problems governed by partial differential equations (PDEs). The surrogate model may be a computationally cheaper alternative to the accurate parameter-to-observable mappings and/or may ignore additional unknowns or sources of uncertainty. The Bayesian approximation error (BAE) approach provides a means to account for the induced uncertainties and approximation errors, i.e. the errors between the accurate parameter-to-observable mapping and the surrogate. The statistics of these errors are, however, in general unknown a priori, and are thus calculated using Monte Carlo sampling. Although the sampling is typically carried out offline, i.e. before considering the data, the process can still represent a computational bottleneck. In this work, we develop a scalable computational approach for reducing the costs associated with the sampling stage of the BAE approach. Specifically, we consider the Taylor expansion of the accurate and surrogate forward models with respect to the uncertain parameter fields either as a control variate for variance reduction or as a means to directly and efficiently approximate the mean and covariance of the approximation errors. We propose efficient methods for evaluating the expressions for the mean and covariance of the Taylor approximations based on linear(-ized) PDE solves. Furthermore, the proposed approach is independent of the dimension of the uncertain parameter, depending instead on the intrinsic dimension of the data, ensuring scalability to high-dimensional problems. The potential benefits of the proposed approach are demonstrated for two high-dimensional inverse problems governed by PDE examples, namely for the estimation of a distributed Robin boundary coefficient in a linear diffusion problem, and for a coefficient estimation problem governed by a nonlinear diffusion problem.

Bayesian approximation error↗

Toxicological Assessment of ISS Air Quality: April - May 2013

A summary of the analytical results from 4 mini-grab sample (mGSCs) collected on ISS and returned aboard 33S is shown in Table 1. Due to the launch delay of the ATV4 resupply mission, monthly samples were reduced in April and May by omitting sampling of the Service Module in order to ensure contingency samplers were available if needed. Complete data tables of all measured concentrations and corresponding T-values based on 180-day SMACs are enclosed. detection limit for all target compounds, except m/p-xylenes and hexachloro-1, 3-butadiene was 0.025 mg/cu m. The detection limit for m/p-xylenes and hexachloro-1, 3-butadiene and all non-target compounds was 0.05 mg/cu m. The average recoveries of the 3 surrogate standards from the mGSCs were as follows: C-13-acetone, 116 +/- 12%; D-5-fluorobenzene, 117 +/- 7%; and D-5-chlorobenzene, 111 +/- 15%. Initial measured sample pressures were between 13.9 and 14.1 psia for all samples, indicating nominal sample collection. A summary of the analytical results from 3 pairs of passive-diffusion formaldehyde badges collected on ISS and returned aboard 33S is also provided in Table 1. In an effort to conserve samples due to the delay of the ATV4 resupply mission, FMK sampling was only conducted in the US Lab in May. Positive control recoveries (1 trip and 2 lab controls) were 79%, 87%, and 116% respectively.

Meyers, Valerie↗

Calibration of the Diffusivity Predictions of Centipede Using Approximate Bayesian Computation and Applications in Nyx (Engineering Scale) and Xolotl-MARMOT (Meso-Scale) Simulations

Fission gas evolution and release in UO 2 nuclear fuel are important fuel performance metrics and occur in several distinct stages: 1) nucleation, growth and resolution of intra-granular bubbles, 2) diffusion to grain boundaries and 3) nucleation and growth of bubbles at grain boundaries, which eventually form a connected network (percolation) enabling release of gas from grain boundaries through connections to triple junctions, grain edges or free surfaces. The NE-SciDAC project is developing several computational tools to model this problem, which are connected in a hierarchical multi-scale framework. The information transfer in the multi-scale framework is a critical step that, in addition to best-estimates, should include uncertainty quantification. Despite taking a first-principles multi-scale approach, there is a need to perform parameter calibration to ensure consistency with available experimental data. In the present study, uncertainty quantification (UQ) and parameter calibration is demonstrated for one of the lower length scale codes in the multi-scale framework (Centipede) and then the results, including instances of the propagated uncertainties, are used in other codes within the framework, specifically Nyx and Xolotl-MARMOT. We calibrated the model parameters in Centipede, a computer code used to predict diffusivities of uranium (U) and xenon (Xe) in the context of the simulation of fission gas in uranium oxide (UO 2 ) nuclear fuel. The Centipede code depends on 183 parameters, all of which are subject to uncertainty. The three data sets used in our calibration effort are taken from the literature. This data is available as a set of measurements, including measurement errors. Our goal is to calibrate a statistical model that predicts both the value of the measurement and the uncertainty associated with the measurement. We perform a Bayesian calibration of the model parameters using a dedicated approximate Bayesian computation (ABC) likelihood function. To avoid excessive computational costs, we replace the expensive Centipede simulation code by a higher-order surrogate model, constructed using only the 9 most important parameters. These important parameters are identified by a preliminary global sensitivity analysis (GSA) study. Among the important parameters are T0 (the temperature at which UO 2 is perfectly stoichiometric) and Hf_pO2 (the temperature dependence of the oxygen (O) partial pressure) that should be considered as operating conditions to be estimated along with the other parameters. We consider two different cases: one where we define one set of these operating conditions for all data sets, and one where we define distinct operating condition parameters for each data set. The Xe diffusivities predicted by the latter case show distinct features that could not be observed in the former. Next, we use the diffusivity predictions by Centipede as input to Nyx, a reduced order fuel performance code focused on gas behavior alone, in order to estimate quantities associated with inter-granular bubble formation at conditions specified by the experiments. Finally, the diffusivities obtained from the calibrated Centipede runs were used in coupled Xolotl-MARMOT simulations of intra- and inter-granular gas evolution. The results are compared to simulations using the baseline diffusivities from Turnbull et al.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Efficient data-driven regression for reduced-order modeling of spatial pattern formation

We present an efficient data-driven regression approach for constructing reduced-order models (ROMs) of reaction-diffusion systems exhibiting pattern formation. The ROMs are learned non-intrusively from available training data of physically accurate numerical simulations. The method can be applied to general nonlinear systems through the use of polynomial model form, while not requiring knowledge of the underlying physical model, governing equations, or numerical solvers. The process of learning ROMs is posed as a low-cost least-squares problem in a reduced-order subspace identified via Proper Orthogonal Decomposition (POD). Numerical experiments on classical pattern-forming systems–including the Schnakenberg and Mimura–Tsujikawa models–demonstrate that higher-order surrogate models significantly improve prediction accuracy while maintaining low computational cost. The proposed method provides a flexible, non-intrusive model reduction framework, well suited for the analysis of complex spatio-temporal pattern formation phenomena.

Data-driven modeling↗

Understanding the ignition process and flame structure of conventional and oxygenated fuels under engine relevant conditions – An optical study

Renewably generated synthetic fuels such as poly-oxymethylene ethers (OME) have a significant potential to effectively break the soot-NOX trade-off in compression ignition engines by using exhaust gas recirculation (EGR) to maintain low nitrogen oxide (NOX) emissions while maintaining good efficiency and simultaneously contributing to circular carbon economy. However, owing to the fundamental differences in properties of OME when compared to fossil-based diesel fuels, it is critical to fully understand its ignition and combustion phenomenology to take advantage of this fuel to its utmost potential. In this context, this work outlines the results of a systematic experimental study performed in a heavy-duty, single-cylinder, optical engine probing the spatial and temporal progression of fuel decomposition and ignition behavior of OME when compared to n-dodecane, a diesel-fuel surrogate. Thermodynamic analysis and optical diagnostics techniques including simultaneous HCHO-PLIF and OH-PLIF complemented by high-speed OH* chemiluminescence were employed along with parametric sweeps of intake temperature and EGR dilution rates. OME does not exhibit any observable low temperature heat release irrespective of the ambient oxygen concentration. Differences in the observed diffusive flame structure such as longer flame lift-off length, less pronounced combustion recession, faster premixed burn at ignition (“volumetric” ignition), non-sooting behavior suggest that the inherent presence of fuel-bound oxygen in OME can skew the air-fuel ratio (AFR) distribution within the jet thereby reducing the reliance of combustion on mixing and air entrainment. This leads to rapid late-cycle oxidation leading to shorter combustion duration and favorable combustion phasing. Results also suggest that OME exhibits relatively weak negative temperature coefficient (NTC) behavior, however, the OME fuel-decomposition kinetic-pathways produce significant concentration of HCHO, which might be erroneously interpreted as a product of cool-flames.

Air-fuel ratio↗

Validation of the HyRAM+ physics models for use with propane

The Hydrogen Risk Assessment Model Plus (HyRAM+) toolkit combines quantitative risk assessment with simulations of unignited dispersion, ignited turbulent diffusion flames, and indoor accumulation with delayed ignition of fuels. HyRAM+ is differentiated from HyRAM in that it includes models and leak data for other alternate fuels. The models of the physical phenomena need to be validated for each of the fuels in the toolkit. This report shows the validation for propane which is being used as a surrogate for autogas, which is a mixture of propane and butane and used in internal combustion engines in vehicles. For flame length comparisons, five previously published experiments from peer reviewed journals were used to validate our models. The validation looked at flame lengths and flame widths with respect to different leak diameters, mass flow rates, and source pressures. Most of the sources included more than one set of experimental data, which were collected using different methods (CCD cameras, IR visualization etc.). In general, HyRAM+ overpredicts the flame lengths by around 65%. For heat and radiation models, we compared the heat flux and radiation data reported from two different sources to the values calculated by HyRAM+. For higher mass flow rates, the HyRAM+ calculated flame length results gave a better estimate of what is found in the experiments (65% error), but a higher error (85%) is observed between the HyRAM+ calculated lengths and the experimental flame lengthsfor lower mass flows. Some differences can be attributed to outdoor environmental effects (i.e. wind speed) and uncertainties in jet flame shapes. The propane flame trajectory is predicted for a high Reynolds number case with Re = 12,500 and a low Reynolds number case where Re = 2,000. The Re=12,500 case which is momentum dominated matches well with the experimental flame trajectory, but the agreement for the bouancy driven low Reynolds number case is not as good. Dispersion modeling for unignited propane was also analyzed. We compared the mole fraction, mixture fraction, mean velocity, concentration half width, and inverse mass concentration over an axial distance from different credible journals to the values calculated by HyRAM+. The results display good agreement but generally, HyRAM+ predicts a wider profile for mole fraction and mixture fraction experiments. Overall, HyRAM+’s results are reasonable for predicting the flame length, heat flux, flame trajectory, and dispersion for propane and can be used in risk analyses

08 HYDROGEN↗

Construction of generalized quasilinear diffusion coefficient using neural networks with physical restrictions

The quasilinear diffusion coefficient (D QL ) derived from our machine learning framework shows comparable trends with the ground truth D QL obtained from GENRAY-CQL3D simulations. Additionally, for the strong absorption cases, the radial current drive profiles generated using the D QL from our model exhibit consistent behavior with those obtained from the original simulation. These findings indicate the potential of our surrogate modeling approach with physical restrictions to replicate key wave–plasma interaction characteristics while reducing computational costs. Traditionally, calculating D QL for wave–particle interactions relies on computationally intensive wave simulations coupled with Fokker–Planck solvers. To address this challenge, we developed a machine learning-based surrogate model with physical restrictions derived from cold plasma theory and bounce-averaged damping effects. First, we establish the propagation domain of Lower Hybrid Waves in the (N∥, ρ) space by identifying the accessibility limit and determining the upper and lower bounds of N∥ using the Potential Power Deposition (PPD) method. Subsequently, leveraging a database constructed using Latin hypercube sampling alongside the underlying physical restrictions (e.g. PPD), machine learning methods including U-Net and Recurrent Neural Networks are employed to design a physics-restricted machine learning framework capable of reconstructing D QL .

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Data‐Efficient Generation of Synthetic Microstructures of Polymer‐Bonded Energetic Material With Fine‐Tuned Stable Diffusion

Among current deep learning approaches for synthetic image generation, diffusion-based models stand out in terms of algorithmic stability and ability to retain high-fidelity image features with detailed resolution. Here, in this work, we employ Dreambooth, a method for fine-tuning Stable Diffusion, on X-ray CT images of microstructure of the polymer-bonded form (PBX) of a commonly used high explosive, Pentaerythritol tetranitrate (PETN), which yields generative models for creating synthetic PBX images. The models developed here represent five classes (or ‘lots’) of microstructures and demonstrate successful generation of images of each class with high fidelity, as verified by computed classification accuracy of ∼ 94% or higher. Data augmentation afforded by such image synthesis can be used to more reliably decipher underlying statistics, build processing-structure correlations, recognize off-normal structural anomalies, and identify age-related changes. Ideas related to converting image data into appropriate density mapping and performing mesoscale simulation or surrogate modeling of detonation are also discussed.

Dreambooth↗

Hydrogen uptake in graphite matrix at high temperature

Tritium management is a critical challenge for the next generation of nuclear reactors, such as Fluoride Salt Cooled High Temperature Reactors (FHRs) and High Temperature Gas-cooled Reactors (HTGRs), due to the higher production rate (up to 10,000 times) than conventional Light Water Reactors (LWRs). Graphitic materials employed as moderator, reflector, and fuel pebbles offer a potential pathway for tritium recovery by serving as a sink for tritium. Prediction of uptake capacity under reactor relevant conditions remains a challenge due to a lack of low partial pressure data and significant inter-grade variability of graphite. This study addresses these gaps by providing a comprehensive characterization of hydrogen (as a tritium surrogate) uptake and release behavior in the A3-3 graphite matrix (GM) used in fuel pebbles. Uptake measurements are performed at reactor relevant temperatures of 600- 800 °C, 1-200 Torr hydrogen pressure, and 15-120 min equilibration time, followed by thermal desorption spectroscopy up to 1100 °C. Uptake experiments at different equilibration times demonstrate the role of kinetics in hydrogen uptake, which can be modeled as a diffusion-with-trapping process. In the thermodynamics limit, the Sips adsorption model is shown to capture the uptake in A3-3 GM well. Our campaign provides a set of new results for hydrogen uptake in A3-3, including limiting uptake capacity at 600 °C, apparent diffusion coefficient at 600 °C, and the first estimates of the FHR/HTGR relevant (600 °C, 20 Pa partial pressure) equilibrium uptake capacity and time to saturation. Desorption data highlights a new site for hydrogen uptake, not observed in nuclear graphite, which we attribute to the non-graphitized binder. Using the Kissinger method, we estimate activation energy for release from the desorption peaks, confirming the activation energy for release from the basal planes and providing the first estimate for the activation energy of release from the binder.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A direct numerical simulation of Jet A flame kernel quenching

The safe operation of aeronautical engines requires an understanding of flame ignition, propagation and extinction. In this study, direct numerical simulations are performed using a 29 species reduced chemical mechanism for jet fuel surrogate Jet A to understand the flame quenching process. Here, initially laminar spherical flames of varying sizes and equivalence ratios are subject to an identical periodic domain of decaying and isotropic high intensity turbulence with a turbulent Reynolds number of 2400. All cases become quenched, except for the larger kernel with lower Karlovitz number. An analysis of the flame structure shows broadened preheat zone, flame shortening on the product side, differential species diffusion and partial fuel pyrolysis in the fresh mixture. Two extinction mechanisms are identified arising from flame shortening and high flame stretch. Flame shortening occurs due to turbulence-chemistry interactions that resemble the flame–flame interaction in a laminar counterflow reactant-to-reactant configuration, which contorts and breaks up the ignition kernel. Flame stretch is a local effect that attenuates the heat release rate and causes the flame to retreat towards the product mixtures, similar to what has been observed for reactant-to-product laminar counterflow flames. Chemical explosive mode analysis was also performed to quantify the flame structure and local combustion mode. The diffusion–reaction balance in pinched-off flame islands favors extinction of these smaller structures, while auto-ignition modes are observed within the flame kernel after fresh mixture is engulfed and preheated in the product kernel. Statistics of the density-weighted displacement speed conditional on local combustion mode indicates strong correlation between the local extinction mode and negative displacement speed. The local balance between diffusion and reaction ultimately determines the propensity for local extinction in both laminar and turbulent flames, the extent of which has an impact on global flame propagation.

42 ENGINEERING↗

Water vapor oxidation of SiC layer in surrogate TRISO fuel particles

Under accidental conditions for high temperature gas-cooled reactors (HTGR), the SiC layer in tri-structural-isotropic (TRISO) fuel particles can be exposed to water vapor. In this study, oxidation behaviors of surrogate TRISO fuel particles were investigated in a He-20 vol% water vapor mixed atmosphere at temperatures up to 1600 °C. The growth of the crystalline oxide passivation layer with cracks and pores followed a parabolic law with time, where the maximum was 2.3 μm at 1600 °C. The oxide layer and the SiC surface under the oxide became flattened with increasing temperature, as a function of the silica viscosity and the diffusion path of water vapor. Volatilization of the oxide layer was analyzed using a mechanistic model that an inert gas in oxidizing atmospheres could influence the magnitude of volatilization. The fracture load and strength of the oxidized and thinned SiC layer were numerically estimated to decrease from 2.27 to 1.69 N and from 317 to 299 MPa, respectively, with the SiC thickness decrease from 35 to 32 μm. This prediction indicates that the oxidized SiC layer should retain fission products. Additionally, the mechanical integrity of each layer in the TRISO fuel particle after oxidation was evaluated. The results in this work provide important data for the safety analysis of accidental scenarios in HTGRs.

36 MATERIALS SCIENCE↗

Effect of sucrose on the oxidation-reduction conditions and retention of rhenium during vitrification of low-activity waste

Technetium speciation and solubility during nuclear waste vitrification are affected by oxygen partial pressure in the melt. Thus, reducing agents such as sucrose, which are routinely added to nuclear waste feeds to repress foaming, can significantly affect the volatilization of Tc and increase its retention in glass. Using Re as a surrogate for Tc, we measured the effect of sucrose addition to two low-activity waste melter feeds on the Re retention, oxygen partial pressure, and iron redox as functions of temperature. As expected, Re retention in glass increased as the sucrose content increased. Furthermore, this is attributed to sucrose reaction with nitrates and nitrites in the feed. Destruction of nitrates and nitrites reduces the salt phase fraction and thus likely promotes Re diffusion into the glass-forming melt. In agreement with available literature, we discuss that a modest increase in the sucrose content (compared to current practice) can significantly improve the Tc retention without reducing Fe 2+ to metal.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗