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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Investigation and Analysis of Dolomite Dissolution in Variable Strength Systems Relevant to the WIPP

The Waste Isolation Pilot Plant (WIPP) was opened in 1999 as a solution to the long-term disposal of the nation's nuclear defense-generated transuranic (TRU) waste. The salt beds were recommended as the ideal location because they are free from flowing fresh water, easily mined, impermeable, and geologically stable. However, for performance assessment modeling, release scenarios must be considered. The most likely release scenario was determined to be human intrusion leading to direct and/or long-term brine release (US DOE 1995, US DOE 1996, Perkins et al., 1999). The focus of this research is the Rustler formation because it is located above the WIPP and is the most transmissive layer (Perkins et al., 1999). Objective: To determine the effect of chelating ligands ( e.g. EDTA) on dissolution of dolomite in high ionic strength systems. Do brines impact dolomite dissolution and how is it affected by EDTA binding with cations? By varying the ionic strengths, different brine conditions can be simulated similar to those in and around the Culebra member and evaluate trends of dissolved Ca and Mg in the aqueous phase from the quantified data. Conclusions: <2% of dolomite dissolved over one week at pH 8.5. Greater dissolution occurred at higher ionic strength and in the presence of NaCl with approximately 0.4 vs. 0.9% of Mg removed from dolomite in 0.1 and 1.0 M Na. Further, 0.3 vs. 0.9% of Mg was removed from dolomite in 1.0 M IS CaCl{sub 2} versus NaCl. EDTA increased dissolution of dolomite at low ionic strength due to its strong complexation affinity for Ca/Mg with slightly greater removal of Ca than Mg. Significant differences were not observed at high ionic strength due to the presence of large concentrations of competing cations (Na, Ca, Mg). Slightly higher concentrations of Ca were removed from dolomite than Mg after one week, suggesting either incongruent dissolution or release through ion exchange of Ca from trace mineral impurities. Further, when EDTA was present, it may have increased Ca removal due to its greater complexation for Ca than Mg. Environmental Implications: High ionic strength brines and low ionic strength solutions with organic ligands increase dissolution of dolomite. Due to the long half-lives of radionuclides in the TRU waste, it may be important to consider the long term impact of dolomite dissolution for potential release scenarios.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Understanding the Dissolution and Passivation of an Aluminum Electrode during Electrocoagulation of Groundwater Using Neutron and X-ray Reflectometry

An aluminum (Al)-based electrocoagulation (EC) system can effectively remove dissolved silica and hardness in groundwater. The effectiveness of Al-EC in terms of pollutant removal, Faradaic efficiency, and energy consumption depends on the interfacial electrolysis or passivation of the electrode in water. Thus, understanding the electrolysis reaction at the liquid/electrode interface during operation is important for sustainable EC deployment. Here, a continuous flow-through Al-EC system was tested with various groundwater simulants, i.e., chloride (Cl – )-based, sulfate (SO 4 2– )-based, and mixed solutions. High pollutant removal with low energy consumption was observed in Cl – -based groundwater treatment, while low pollutant removal with high energy consumption was observed in SO 4 2– -based groundwater. For example, the required energy per unit mass of Al dosing in SO 4 2– -based groundwater is three times higher than that in Cl – -based groundwater at 10 mA/cm 2 . However, increasing the Cl – concentration significantly reduces this energy demand. In SO 4 2– -based groundwater, the silicate removal efficiency drops from 85.1% to 24.0% compared to that for Cl – -based groundwater, while Mg 2+ and Ca 2+ removal efficiencies decrease to 0.6% from 15.8% and 5.7% from 44.8%, respectively. To better understand this EC performance, we used in situ neutron reflectometry (NR) to examine the interfacial dynamics of Al dissolution and passivation at a 100 nm scale occurring on the surface of the sacrificial Al electrodes during EC. Ex situ X-ray reflectometry (XRR) was also used to support the in situ NR results. Both NR and XRR results revealed that Al dissolution is influenced by the presence of Cl – in the simulants, while a passivating layer forms on the electrode in a SO 4 2– -based solution. In the Cl – -based solution, anodic Al dissolution occurred locally and inhomogeneously across the surface of the Al anode film, resulting in a localized thickness reduction over time. In the SO 4 2– -based solution, no apparent dissolution of the Al anode was identified. Instead, Al underwent oxidation, forming an amorphous Al 2 O 3 surface layer within the Al electrode film that increased in thickness over time. In the mixed solution, both anodic Al dissolution and surface Al 2 O 3 layer formation occurred, indicating that Al dissolution and surface Al 2 O 3 layer formation are attributable to the Cl – and SO 4 2– ions, respectively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Dissolution and initial hydration behavior of tricalcium aluminate in low activity sulfate solutions

Influences of alkali or alkaline earth sulfates on the hydration of cubic tricalcium aluminate (C 3 A) were evaluated by in situ dissolution rate measurements, by ex situ near-surface composition measurements with secondary ion mass spectrometry, and by in situ synchrotron X-ray diffraction to monitor precipitation of hydration products. Both slight reductions in dissolution rate and cation-specific interactions with the solid were observed. The near-surface Ca/Al ratio is significantly lower after some dissolution and the electrolyte cations are incorporated within the surface with different affinities (Mg 2+ > K + > Na + ). An interfacial dissolution-reprecipitation mechanism may explain the observations as well as, or better than, a simple cation exchange. The sulfate concentration in solution affects the rates of both C 3 A dissolution and precipitation of hydration products. Aditionally, sulfate ions likely adsorb at the hydrous Al-rich surface layer, thereby reducing the dissolution rate of aluminates and delaying the precipitation of aluminate hydration products.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Mechanisms and kinetics of citrate-promoted dissolution of a uranyl phosphate mineral

The formation of uranyl phosphate precipitates is a remediation strategy to limit the mobility of uranium in contaminated soils. However, exposure to organic ligands, like the plant exudate citrate, can remobilize the uranium. The purpose of this study is to provide a more thorough comprehension of citrate-promoted dissolution of a uranyl phosphate mineral, chernikovite [(H 3 O)(UO 2 )(PO 4 )·3H 2 O], by determining the extent of uranium release from chernikovite at a wide range of citrate concentrations. Here we have quantified the kinetics of dissolution and proposed potential mechanisms of chernikovite dissolution to gain a better understanding of the fate of uranyl phosphate precipitates in the environment. Batch dissolution and continuously stirred tank reactor (CSTR) experiments indicate that increasing citrate concentrations from 0.1 mM to 50 mM increases the concentration of dissolved uranium. However, at citrate concentrations of 10 mM and greater, the effectiveness of the ligand to enhance the dissolution decreases. Density functional theory modeling and Raman spectroscopy indicate a strong interaction between citrate and the uranyl ions at the surface of the uranyl phosphate. The interaction between citrate and uranyl suggests the formation of an alteration layer of uranyl-citrate surface complexes, which could impede uranium release at citrate concentrations of 10 mM or higher. Together, these results indicate that the citrate-promoted dissolution of chernikovite is a fast reaction that is hindered by a combination of surface saturation and a secondary-phase precipitation reaction at higher concentrations of citrate and reaction times greater than or equal to 72 min based on the hydraulic residence time of CSTR experiments. These findings improve our understanding of the stability of uranyl phosphate for use in sequestration of uranium groundwater plumes at contaminated sites.

58 GEOSCIENCES↗
DOE OSTI2024

The effect of cerium, neodymium, and ytterbium doping on UO 2 dissolution

Here, the dissolution rate of spent nuclear fuel has been studied heavily to understand the impacts of a failed waste package scenario on potential radionuclide release from a geologic repository. Multiple countries have evaluated these scenarios in oxidizing and reducing environments respective to their relevant repository conditions. The repository environment (e.g., water chemistry, temperature, oxygen content) and the fuel itself (e.g., chemical content of the fuel) both heavily impact the dissolution rate of the spent fuel. This work examined the impact that rare earth element dopants (Ce, Nd, Yb) have on the fuel dissolution under repository relevant conditions with decreasing oxidizing conditions using a single pass flowthrough system. UO 2 samples were doped with Ce, Nd, or Yb with concentrations between 1 and 5 at%. The addition of dopants to the samples reduced the dissolution rates on most samples relative to pure UO 2 samples. Scoping experiments that occurred in a less oxidizing environment showed a reduction in dissolution rate compared to fully oxidizing conditions. The results within highlight the importance of dopant behavior in used fuel dissolution modeling.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Radiolysis and Radiation-Driven Dynamics of Boehmite Dissolution Observed by In Situ Liquid-Phase TEM

We report over the last several decades, there have been several studies examining the radiation stability of boehmite and other aluminum oxyhydroxides, yet less is known about the impact of radiation on boehmite dissolution. Here, we investigate radiation effects on the dissolution behavior of boehmite by employing liquid-phase transmission electron microscopy (LPTEM) and varying the electron flux on the samples consisting of either single nanoplatelets or aggregated stacks. We show that boehmite nanoplatelets projected along the [010] direction exhibit uniform dissolution with a strong dependence on the electron dose rate. For nanoplatelets that have undergone oriented aggregation, we show that the dissolution occurs preferentially at the particles at the ends of the stacks that are more accessible to bulk solution than at the others inside the aggregate. In addition, at higher dose rates, electrostatic repulsion and knock-on damage from the electron beam causes delamination of the stacks and dissolution at the interfaces between particles in the aggregate, indicating that there is a threshold dose rate for electron-beam enhancement of dissolution of boehmite aggregates.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Effect of Adsorbed Carboxylates on the Dissolution of Boehmite Nanoplates in Highly Alkaline Solutions

Understanding the dissolution of boehmite in highly alkaline solutions is important to the processing of the complex nuclear wastes stored at the Hanford (WA) and Savannah River (SC) sites. Here, we report the adsorption of model carboxylate anions on boehmite nanoplates in alkaline solutions and their effects on subsequent boehmite dissolution in 3 M NaOH at 80 °C. Although expectedly lower than at circumneutral pH, adsorption of oxalate at pH 13 at room temperature was significant and remained so through a linear decrease to 3 M NaOH conditions with no evidence for the appearance of new phases. Modeling of the adsorption data and rate were consistent with the formation of outer-sphere surface complexes. By using these conditions to preload the boehmite nanoplates with oxalate, and separately acetate, we measured and compared their dissolution behavior at 80 °C and observed a clear suppression of the dissolution rate for the case of adsorbed oxalate by 23% and for adsorbed acetate by 10% compared to pure solids. Ex situ scanning electron microscopy (SEM) and transmission electron microscopy (TEM) characterization revealed no detectable difference in the morphologic evolution of the dissolving boehmite materials. In conclusion, we nonetheless conclude that pre-adsorbed carboxylate anions, even as nominally weakly bound outer-sphere complexes, can persist on the surface through highly alkaline conditions, decreasing the density of dissolution-active sites and thereby adding an extrinsic control on the dissolution rate.

Adsorption kinetics↗
DOE OSTI2020

An Atomic-Scale Understanding of UO 2 Surface Evolution during Anoxic Dissolution

Our present understanding of surface dissolution of nuclear fuels such as uranium dioxide (UO 2 ) is limited by the use of non-local characterization techniques. In this paper, we discuss the use of state-of-the-art scanning transmission electron microscopy (STEM) to reveal atomic–scale changes occurring to UO 2 thin films subjected to anoxic dissolution in deionised water. No amorphisation of the UO 2 film surface during dissolution is observed, and dissolution occurs preferentially at surface reactive sites that present as surface pits which increase in size as the dissolution proceeds. Using a combination of STEM imaging modes, energy-dispersive X-ray spectroscopy (STEM-EDS), and electron energy loss spectroscopy (STEM-EELS), we investigate structural defects and oxygen passivation of the surface that originates from the filling of the octahedral interstitial site in the centre of the unit cells and its associated lattice contraction. Taken together, our results reveal complex pathways for both the dissolution and infiltration of solutions into UO 2 surfaces.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Refinement of Salt Dissolution Inhibitor Requirements (Final Report)

At Savannah River Site (SRS), High-Level Waste is stored in below-grade carbon steel tanks. This waste in part consists of sludge, salt cake, and/or supernate. Preparation of this waste for future processing involves dissolution of the salt cake layer. The salt dissolution process can create conditions that leave the carbon steel tanks susceptible to localized corrosion. The salt to be dissolved contains high concentrations of nitrate, that once released, create an environment that may be conducive to pitting corrosion and/or stress corrosion cracking (SCC) of carbon steel. The salt dissolution process also liberates interstitial liquid trapped between the salt crystals. This liquid is initially high in nitrite and hydroxide concentration. High pH and greater ratios of nitrite to nitrate act as inhibitors to minimize corrosion of carbon steel in high nitrate environments. However, as dissolution proceeds, the concentration of nitrate will increase, while the hydroxide and nitrite concentration of the interstitial liquid will deplete and become insufficient to prevent the onset of corrosion attack. Tank blending and addition of inhibitors are used to ensure adequate concentrations of hydroxide and nitrite. However, this is not desirable during salt dissolution as it can reduce process efficiency and increase the amount of waste that needs processing. It has been proposed that these corrosion control limits be revisited to evaluate the corrosion susceptibility of carbon steel in environments that more closely resemble current operating conditions at SRS. An experimental matrix was designed to evaluate the use of the pitting factor for supernate chemistries characteristic to SRS, particularly during the salt dissolution process. Two electrochemical methods were identified to determine the susceptibility of A537 and A285 low-carbon steels to pitting corrosion with this chemistry envelope at temperatures up to 75 °C. The predominant electrochemical test method was Cyclic Potentiodynamic Polarization (CPP) studies. Through CPP, the pitting factor was used, based on Hanford Site corrosion studies, to accurately identify pitting susceptibility within the compositional range studied with some conservatism. Additionally, sulfate was determined to have no statistically significant influence, at concentrations up to 0.6 M, on pitting behavior in more concentrated solutions where other aggressive species govern pitting susceptibility. Where CPP was inconclusive, Modified ASTM G192 was successfully used to evaluate pitting susceptibility conditions and allowed for a pass/fail result to be determined. In all cases, the pitting factor was determined to be applicable to the simulants tested, with this metric accurately predicting incidences in which pitting occurred. Based upon the findings in this work, a pitting factor of 1.2 is being proposed to build in a safety factor and remain consistent with the Hanford Site approach. Additionally, a minimum pH limit of 12 is proposed to ensure carbon steel passivity and localized corrosion the primary degradation mechanism. Susceptibility to SCC was evaluated using a reduced matrix of tests at 75 °C. No failures due SCC were observed at open circuit. In addition, tests polarized anodically by 200 mV only resulted in failures for trials with pitting factors less than 0.86. However, a test with a passing condition based upon the pitting factor metric (pitting factor = 1.40) did exhibit a failure with an applied potential of +300 mV vs. OCP. This result is contrary to the prediction based upon the pitting factor, however, a polarization of 300 mV, or even 200 mV, from open circuit is substantial. The relationship between these testing parameters and service environment/conditions and the desired level of conservatism in the metric should be further evaluated in the determination of the significance of this result. While the pitting factor accurately predicted susceptibility to SCC at temperatures up to 75 °C and with positive overpotentials up to 200 mV, the relatively small sample matrix and failure of a passing pitting factor with a 300 mV polarization resulted in an inconclusive determination of whether the pitting factor may be used for predicting susceptibility to SCC at temperatures between 50 °C and 75 °C. As such, additional testing is recommended to evaluate the validity of the pitting factor for SCC susceptibility prediction at temperatures between 50 °C and 75 °C.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Environmental and economic analyses of chemical recycling via dissolution of waste polyethylene terephthalate

Globally, more than 1000 organizations and 175 nations are facing the plastic waste problem and have realized the need to transition from “linear-to-circular” economy of plastics. While the current mechanical recycling technologies for plastics are struggling to increase the U.S. plastic recycling rates beyond 9%, chemical recycling technologies become important complementary technologies to the predominant mechanical recycling that are needed to realize the circular economy in plastics supply chains. Dissolution is one such chemical recycling technology that can recycle waste plastic back into high-quality virgin grade plastic. However, the environmental and economic impacts of chemical recycling of waste polyethylene terephthalate (PET) via dissolution technology using a green solvent are unknown. Our study evaluated environmental metrics such as greenhouse gas (GHG) emissions and cumulative energy demand, and economic metrics such as net present value (NPV), minimum selling price, payback period, return on investment, and discounted internal rate of return for three dissolution processes with polymer recovery via anti-solvent, evaporation, and cooling precipitation techniques. The dissolution process with evaporation technique was the most economically favorable, whereas that with cooling technique was the most environmentally favorable. The anti-solvent approach had low economic performance and the highest environmental impacts. The NPV for all of these technologies ranged from $2.67 MM to $10.93 MM for a capacity of 8,400 MT/year and was found to be the highest for dissolution with evaporation approach and the least for anti-solvent approach. The cradle-to-gate GHG emissions and energy demand for PET dissolution processes ranged from 1.33-3.77 kg CO2-eq/kg of chemically recycled (CR) PET and18.9-56.1 MJ/kg of CR-PET, respectively. These economic and environmental metrics will be helpful in evaluating the sustainability of circular PET supply chains in the U.S.

09 BIOMASS FUELS↗
DOE OSTI2021

Rapid dissolution of PuO 2 analytical samples using mediated electrochemical oxidation

Current methods for quantitative dissolution of solid PuO 2 involve lengthy dissolution times. The adaptation of mediated electrochemical oxidation, which uses an electrochemically produced oxidizing agent to catalyze dissolution, has been explored for radiochemical analysis scale dissolutions of PuO 2 . The effects of temperature, electrode material, and electrocatalyst on the dissolution kinetics were explored. Under conditions examined in this study, complete dissolution of tens of milligrams of solid PuO 2 can be achieved in less than 1 h at ambient temperature. Overall, this methodology could be adapted to dissolve other metal oxides.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Metal dissolution from first principles: Potential-dependent kinetics and charge transfer

Metal dissolution and its inverse process are integral to both corrosion and electrodeposition; however, many mechanistic details regarding the dissolution process are challenging to decipher. These include how ion dissolution kinetics and charge transfer are influenced by the competition between metal and solvent interactions under an electrode potential. Here, in this work, we introduce a computational framework based on density functional theory with grand-canonical treatment of electrons to directly predict the potential energy landscape for metal dissolution at a constant potential. Using aluminum as an example, we demonstrate that dissolution kinetics is governed by competing kinetics between two physical processes associated with metal–metal bond breaking and ion-migration within the electrical double layer, respectively. We identify a kinetic transition between regimes dominated by each of these processes and show that this transition depends on the operating electrode potential, among other key factors. It is further found that kinetics and thermodynamics of these processes can be described with a simple, one-parameter Marcus-theory-type model. Beyond offering new understanding of charge transfer during dissolution, our simulation protocol provides a recipe for directly predicting other important quantities in electrochemical reactions from first principles that are difficult to measure, such as the symmetry factor.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Impacts of Permeability Heterogeneity and Background Flow on Supercritical CO 2 Dissolution in the Deep Subsurface

Motivated by CO 2 capture and sequestration (CCS) design considerations, we consider the coupled effects of permeability heterogeneity and background flow on the dissolution of a supercritical CO 2 lens into an underlying deep, confined aquifer. We present the results of a large-scale Monte Carlo simulation study examining the interaction of background flow rate and three parameters describing multi-Gaussian log-permeability fields: mean, variance, and correlation length. Hundreds of high-resolution simulations were performed using the PFLOTRAN finite volume software to model CO 2 dissolution in a kilometer-scale aquifer over 1,000 years. Predictive dimensionless scaling relationships relating CO 2 dissolution rate to heterogeneity statistics, Rayleigh (Ra) and Péclet (Pe) numbers were developed for both gravitationally dominated free convection to background flow-dominated forced convection regimes. An empirical criterion, Pe = Ra 3/4 , was discovered for regime transition. All simulations converged quickly to a quasi-steady, approximately linear dissolution rate. However, this rate displayed profound variability between permeability field realizations sharing the same heterogeneity statistics, even under mild permeability heterogeneity. In general, increased heterogeneity was associated with a lower mean and higher variance of dissolution rate, undesirable from a CCS design perspective. The relationship between dissolution rate and background flow was found to be complex and nonlinear. Dimensionless scaling relationships were uncovered for a number of special cases. Results call into question the validity of the Boussinesq approximation in the context of modest-to-high background flow rates and the general applicability of numerical simulations without background flow.

42 ENGINEERING↗
DOE OSTI2022

Effect of grain dissolution on sloping ground

The static and dynamic stability of natural or constructed slopes can be affected by dissolution or dissolution-like phenomena. Their underlying mechanisms, however, remain unclear. New experimental results and discrete element simulations provide particle-level and macroscale information on the consequences of mineral dissolution on slope behavior. At the microscale, load-carrying grain arches develop around dissolving particles, the porosity increases, and contact force chains evolve to form a honeycomb topology. At the macroscale, while vertical settlements are the prevailing deformation pattern, lateral granular movements that create mass wasting are prominent in sloping ground, even under the quasi-static granular loss. Horizontal grain displacement is maximum at the surface and decreases linearly with the distance from the slope surface to become zero at the bottom boundaries, much like vertical granular displacement along the depth. Sediments with smaller friction angles and steeper slopes experience greater displacement, both vertically and horizontally. Slopes become flatter after dissolution, with the reduction in slope angle directly related to the loss in ground elevation, ΔH/H o . Yet, because of the porous fabric that results from dissolution, vertical shortening is less than the upper bound, estimated from the loss in the solid mass fraction, ΔH/H o ≈SF. Under water-saturated conditions, the post-dissolution fabric may lead to sudden undrained shear and slope slide.

42 ENGINEERING↗
DOE OSTI2023

Atomic-scale modeling of the dissolution of oxidized platinum nanoparticles in an explicit water environment

Pt nanoparticles (NPs) are currently being investigated for use in fuel cells; however, Pt NP oxidation as a function of size, morphology, and temperature is not well understood or currently quantified. In this study, the stability and dissolution of oxidized platinum NPs is examined via classical molecular dynamics in an explicit water environment. The NPs considered range in size from 1.35 to 2.92 nm in diameter and included five different monolayer (ML) coverages of O*. The simulations were performed at 300, 450, and 600 K with the many-body, reactive third-generation charge-optimized many-body or COMB3 potentials and examine the kinetics of NP dissolution in water. The Pt–O layer, which reduces the kinetic activity for Pt atom dissolution, is projected to make dissolution more favorable for O* MLs smaller than 0.5. The simulations further indicate that the Pt NPs' kinetic rates of dissolution are slowed by an increase in the number of adsorbed species caused by the dissociation of water molecules at the reconstructed facets of the Pt NPs. Furthermore, these findings quantify the effect of oxygen and temperature on the stability and dissolution of oxidized platinum NP in an explicit water environment similar to the conditions in fuel cells and electrocatalysis.

08 HYDROGEN↗
DOE OSTI2020

Fracture, Dissolution, and Cementation Events in Ordovician Carbonate Reservoirs, Tarim Basin, NW China

Ordovician carbonate rocks of the Yijianfang Formation in the Tabei Uplift, Tarim Basin, contain deeply buried (>6000 m), highly productive oil and gas reservoirs associated with large cavities (>10 m). Previous workers inferred that large cavities are paleocaves (paleokarst) formed near the surface and subsequently buried. Alternately, caves may have formed by dissolution at depth along faults. Using 227 samples from 16 cores, we document textures and cement compositions bearing on cavity histories with petrographic, high-resolution scanning electron microscopy (SEM), isotopic, and fluid inclusion microthermometric observations. Results show that dissolution occurred at depth and was caused by (1) acidic fluids derived from Middle-Late Silurian and/or Devonian-Permian hydrocarbon generation and maturation, (2) high-temperature fluids, of which some were associated with Late Permian igneous activity, and (3) Mg-rich fluids that accompanied Jurassic-Cretaceous deformation and the formation of partially open fractures and stylobreccias (fault breccias). The relative paragenetic sequence of the structure-related diagenesis suggests seven stages of fracturing, dissolution, and cementation. Mottle fabrics in the Yijianfang Formation contain argillaceous carbonate-rich silt and are bioturbation features formed within the marine environment. Those mottled fabrics differ from clearly karstic features in the overlying Lianglitage Formation, which formed by near-surface dissolution and subsequent infilling of cavities by allochthonous sediment. Mottle fabrics are crosscut by compacted fractures filled with phreatic-vadose marine cements and followed by subsequent generations of cement-filled fractures and vugs indicating that some fractures and vugs became cement filled prior to later dissolution events. Calcite cements in fractures and vugs show progressively depleted values of δ18O documenting cement precipitation within the shallow (~220 m), intermediate (~625 m), and deep (~2000 m) diagenetic environments. Deep (mesogenetic) dissolution associated with fractures is therefore the principal source of the high porosity-permeability in the reservoir, consistent with other pieces of evidence for cavities localized near faults.

58 GEOSCIENCES↗
DOE OSTI2021

Residual Insoluble Solids Expected from Saltcake Dissolution

A review of previous SRS saltcake dissolution and characterization studies was performed to inform the analysis of the amount of residual insoluble solids that may result from saltcake dissolution. A realistic value covering most cases for the maximum volume of a settled layer of residual insoluble solids that would result from dissolution of a volume of saltcake was calculated as 0.08 mL/mL (8 vol%). Applying factors to account for dissolution test uncertainty and differences between in-tank settling and laboratory testing, the recommended value for a settled layer of residual insoluble solids that would result from dissolution of a volume of saltcake is 0.16 mL/mL (16 vol%). This should apply to dissolution of saltcake with typical minimal amounts of entrained sludge but may not apply to saltcake with significant sludge. As it is composed of primarily non-radioactive isotopes, the precipitated aluminum hydroxide material does not contribute to the heat load.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Acid Dissolution Behavior of Ferritic FeCrAl Tubes Candidates for Nuclear Fuel Cladding

The international materials community is engaged in finding safer alternatives to zirconium alloys for the cladding of fuel in light water reactors. One solution is to replace the zirconium cladding using ferritic iron-chromium-aluminum (FeCrAl) alloys, which offer extraordinary resistance to high-temperature reaction with air or steam due to the formation of a protective alumina layer on the external surface. It is important to characterize the behavior of FeCrAl not only during accident conditions but in the entire fuel cycle, which may include reprocessing of the used fuel after it is removed from the power reactors. The reprocessing may involve the dissolution of the fuel rods in mineral acids. Little or nothing is known on the dissolution of FeCrAl alloys in common mineral acids, therefore the objective of this research was to study the dissolution of typical cladding tubing having two compositions of FeCrAl (APMT and C26M) in three acids (H 2 SO 4 , HNO 3 , and HCl) as a function of the temperature using both standard ASTM immersion tests as well as electrochemical tests. The dissolution behavior of the FeCrAl alloys is compared to the dissolution capability of other traditional nuclear materials such as austenitic stainless steels (304SS and 316SS) and austenitic nickel alloys (Alloy 600 and Hastelloy C-276). Results show that both C26M and APMT have a higher dissolution capability in the studied mineral acids, which will be beneficial for reprocessing procedures.

36 MATERIALS SCIENCE↗