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NASA NTRSDate not supplied

Impact of General Aviation Operations on Airport Performance Through Fast-Time Simulations at Charlotte Douglas International Airport

NASA, in partnership with the Federal Aviation Administration and commercial airlines, deployed the Integrated Arrival, Departure, and Surface (IADS) traffic management system at Charlotte Douglas International Airport (CLT) in 2017 for field evaluation. The system features new capabilities of data exchange and integration, collaborative surface metering and scheduling, which has demonstrated operational benefits of reducing delay time and fuel consumption. General Aviation flights, however, are not currently included in the surface metering programs because of their different operational procedures and lack of reliable predictability in departure time. Thus, their impact on the system performance is not well understood. This paper presents a study of the impact of General Aviation traffic at CLT using fast-time simulations.

General Aviation↗

NASA NTRSDate not supplied

The System Complexity Metric (SCM) Predicts System Costs and Failure Rates

A complex system has many parts and interactions and so is difficult to understand. Systems with higher complexity generally have higher costs and failure rates. A System Complexity Metric (SCM) is defined to be the sum of the number of nodes, N, in the system block diagram plus the number of one-way interactions, I, between the nodes. SCM = N + I. SCMs are easily determined by direct inspection of high level block diagrams of life support systems. System cost was found to be directly proportional to SCM. The system MTBF (Mean Time Before Failure) is the inverse of the system failure rate. MTBF = 1/f. The system MTBF was found to be proportional to SCM^(-2.2) for estimated preflight MTBFs. As is typical for systems that are not extensively tested and redesigned to eliminate unexpected failure modes, the life support flight failure rates were about ten times higher than the preflight estimates and the MTBFs one-tenth the preflight estimates. The system MTBF was found to be proportional to SCM^(-2.6) for observed flight MTBFs.

System compleity↗

NASA NTRS2021

Large-Eddy Simulation of Variable Speed Power Turbine Cascade with Inflow Turbulence

Numerical results are presented from theNASAGlenn Research Center’sin-house turbomachinery code, Glenn-HT applied to the Variable Speed Power Turbine (VSPT) experiment at the NASA Transonic Turbine Blade Cascade Facility.The main goal of this paper is to implement a digital filtering method to generate turbulence upstream and a sub-grid model (Localized dynamic k-equation model (LDKM)) in the framework of LES in order to investigate the effect of inflow turbulence on the transition seen in the VSPT experimental data at the cruise condition (incidence angle of 40oand Tu = 0.5%, 5%,10%, and 15%). Although the boundary layer on thesuction side and pressure side of the blades is initially laminar due to favorable pressure gradient, the laminar flow can transition to turbulent flow past a separation zoneon the suction sideor by natural or by-pass transition. This process determinesthe total-pressure lossesin the wake. Therefore, it is desirable to develop a reliable prediction tool to accurately capture the transition mechanism in blade rows operated under the conditions of low Reynolds number andat a variety offree stream turbulence conditions. Our numerical studies reveal that the location of separationis rather insensitive to the level of Tu, however the effect ofincreasingTu seems to be in reducing the size and ultimately suppressing the separation bubble. In addition, we performedspectral analysis to identify the peak frequencies in the region where the separation bubble is formed, which provides valuable insights into the transition/separation mechanism.

CFD↗

NASA NTRSDate not supplied

Experimental, Computational, Theoretical and Analytical Investigation of Flow Boiling in Reduced Gravity

Two-phase thermal management systems are far superior to their single-phase counterparts because of their ability to capitalize on the coolant’s both sensible and latent heats, thereby yielding orders of magnitude higher heat transfer coefficients and smaller system footprints. A vital knowledge necessary for their implementation in future space systems is performance in microgravity. Long-duration microgravity experiments are necessary to obtain reliable databases, which would then be used to build reliable predictive tools. To achieve this goal, investigators at the Purdue University Boiling and Two-Phase Flow Laboratory (PU-BTPFL) and the NASA Glenn Research Center (NASA-GRC) have been collaborating towards the development of the Flow Boiling and Condensation Experiment (FBCE) and eventual execution onboard the International Space Station (ISS). FBCE has now matured to a point where it is ready for transport to the ISS, where first tests will be conducted using the Flow Boiling Module (FBM). In preparation for the ISS tests, a series of pre-launch Mission Sequence Tests (MSTs) was performed at GRC in Earth gravity with FBM mounted in a vertical upflow orientation using n-perfluorohexane as working fluid. The pre-launch tests included variations of flow rate, surface heat flux, inlet conditions, and both single-sided and double-sided wall heating. This presentation will summarize experimental results from these tests as well as both analytic and theoretical tools for prediction of two-phase heat transfer coefficient and critical heat flux (CHF). Also discussed will be an assessment of predictive accuracy of these tools against the experimental data.

Mission Sequence tests↗

NASA NTRS2021

Orion Meteoroid and Debris Analysis with a Single Kevlar® Layer Enhancement to the Propulsion Tank Multi-Layer Insulation: Comparison of the Observed Data and the Adjusted Ballistic Models

In a continual mass optimization effort for the Orion vehicle by NASA and its prime contractor Lockheed Martin Space, along with the European Space Agency (ESA) and its contractors Airbus and Thales Alenia Space-Italy (TAS-I), a series of shield characterization shots have been performed to quantify the ballistic enhancement of a single-layer of Kevlar® in multi-layer insulation (MLI). This enhanced MLI is part of Orion’s propulsion subsystem, and it is planned to replace a double-layer Kevlar® configuration starting at the Artemis IV mission. This effort has included fifty-two shield characterization shots for five different shield configurations over the four Orion propellant storage vessels. These storage vessels are located in the European Service Module (ESM). This shield characterization has been managed by the Hypervelocity Impact Technology (HVIT) group in NASA Astromaterials Research and Exploration Sciences at Johnson Space Center (JSC) for the NASA Engineering and Safety Center (NESC) and the Multi-Purpose Crew Vehicle (MPCV) program office in coordination with Lockheed Martin Space and Thales Alenia Space-Italy (TAS-I). The shield characterization has used the two-stage, light-gas-gun at the Remote Hypervelocity Test Laboratory (RHTL) of NASA JSC White Sands Test Facility (WSTF) for acceleration of projectiles to representative orbital impact speeds. From this shield characterization effort, a revised ballistic limiting equation (BLE) has been developed for each of the five representative shielding configurations of the ESM pressure vessels. This document provides a brief description of the shield configurations considered for the Orion program and the shield characterization findings. These results are compared to the assumed BLE for each configuration going into the Artemis missions that utilize this version of ballistic enhanced MLI. The models are integrated into a fourteen day High Lunar Orbit (HLO) mission as a representative reliability prediction impact for Orion, and it has been found that the predicted risk of a loss-of-crew (LOC) event is actually a little less than half of the assumed value that launched this design modification opportunity.

Joshua E Miller↗

NASA NTRSDate not supplied

Advancement of Entry System Modeling to Support Exploration of Giant Planets

This paper describes NASA’s efforts to advance entry system modeling and simulation capabilities to support future exploration of Giant planets. The Giant planets are key destinations of interest to the planetary science community for their potential to provide insight into the formation and evolution of our Solar System, as well as extrasolar planetary systems. To date, the Galileo atmospheric probe is the only purpose-built entry probe to a Giant planet. Post-flight analysis of Galileo’s performance showed that there was significant recession of the thermal protection system (TPS), well beyond what was anticipated on the flank, and this was due in part to insufficiently accurate capability for estimating the flight environment and TPS response. While Galileo ultimately survived its flight, the example serves to highlight the great challenge of designing successful missions for environments that are poorly understood or where models have not yet been validated. An important means to reduce mission risks is the incorporation of physics-based modeling with well-quantified uncertainties. The emphasis on physics-based modeling – in contrast to empirically-driven models – is motivated by the fact that it is impossible to completely replicate entry environments through ground tests and, therefore, extrapolation to the flight environment is required. Basing analysis in fundamental physics removes the bias of ground test limitations, though one must then be careful to properly characterize model inputs, simplifying assumptions, and the limits wherein the model is valid. NASA’s Entry Systems Modeling (ESM) Project is tasked with investigating such considerations for planetary science missions across the Solar System, and in recent years has begun to do so for Giant planets. The most distinctive features of the Giant planets, from an entry system perspective, are the atmospheres composed primarily of hydrogen and helium. The entry velocities of proposed missions are generally very large and can therefore be expected to result in significant convective and radiative heating generated by the vehicle’s shock layer. Yet thermochemical behavior of the hydrogen-helium system is not well understood under such conditions. The ESM project is leading efforts to develop accurate thermochemical databases based on state-of-the-art measurements in the Electric Arc Shock Tube and detailed computational chemistry. The large heat fluxes anticipated by missions has driven interest in new TPS materials, in particular woven materials, which may be enabling but have never been flown before. Consequently, multiscale models are in development to describe properties and performance of the materials from micro- to system-scale. The goal is to not only provide accurate thermal response but also to inform thermostructural reliability predictions for extreme entries. Additionally, new computational models have been developed to evaluate performance of non-destructive evaluation techniques which are vital to establishing acceptance of systems to be free of manufacturing faults like material cracking, voids, and debonding. Finally, in the area of guidance and control, aerocapture has been shown conceptually to provide a number of mission benefits, including reducing transit time and increasing payload fraction. The ESM project is building a launch-to-landing trajectory simulation capability to enable detailed studies of aerocapture maneuvers in the context of Giant planets missions. The final presentation and paper will describe each of these topics in detail, including discussion of specific gaps and the technical approach to solving them. In addition, the final paper will briefly discuss ongoing coordination between ESM project work and an ESA-funded technology development activity comprised of validation testing in the Oxford T6, IRS PWK and IST ESTHER tunnels, as well as state-to-state modeling of the shock layer to better represent non-Boltzmann energy distributions leading to non-equilibrium radiation.

Entry systems↗

NASA NTRS2020

Exploring the Limits of the Data-Model-Theory Synergy: “Hot” MW Transitions for Rovibrational IR Studies

In order to further improve the accuracy of rovibrational IR line lists generated from the “Best Theory +Reliable High-resolution Experiment” (BTRHE) strategy from 0.01-0.05 cm-1, or 300-1500 MHz, to ~10 MHz, we explore the current limits of the Data-Model-Theory synergy by examining the accuracy and consistency of existing data, then propose that “hot” bands in microwave (MW) spectra is the solution we need for future enhancements. The Ames SO2 J=0-20 rovibrational energy levels computed on the semi-empirically refined Ames-2 potential energy surface (PES) are fit to the Effective Hamiltonian (EH) model regularly used in the experimental infrared (IR) analysis for SO2 isotopologues. In the fitted EH(Ames) model, the rotational constants A/B/C and all 5 quartic centrifugal distortion constants display clear, systematic, and consistent patterns along the vibrational state energy or quanta. Such consistent patterns may facilitate the vibrational assignments for MW hot bands and extract more information from high temperature MW spectra. Some EH(Expt) analyses were carried out with the lowest order Coriolis Coupling term, C1. Their constants should not be directly compared with other EH(Expt) and EH(Ames) results. After excluding them, our  = EH(Ames)- EH(Expt) analyses for 5 isotopologues (626, 636, 646, 628 and 828) indicates some loss of accuracy and consistency starting from vibrational states as low as 22 or 1000 cm-1. Some EH parameters, e.g. K, may have relative deviations as large as 50-100% and totally lose any recognizable patterns. This simply means that current EH(Expt) models do not have the system-wide consistency we need to further refine the EH(Ames) and Ames rovibrational IR line lists. A large part of such defects are probably inherited from the limited precision of experimental line positions, i.e. 1E-3 ~ 1E-4 cm-1, or 3-30 MHz. This is confirmed in a series of truncation tests using the Ames data. Although the EH(Ames) consistency may help identify unreliable rovibrational EH(Expt) parameters, and make reliable predictions for minor isotopologues and unobserved vibrational bands, we believe only the highly accurate “hot” MW transitions can provide real enhancements for EH(Expt) accuracy and consistency. “Hot” MW spectra should play a more significant role in the future synergy of Data, Model, and Theory in the field of rovibrational IR studies.

Xinchuan Huang↗

NASA NTRSDate not supplied

Fan Acoustic Flight Effects on the PAA & ASN Flight Test

Accurate and reliable prediction of noise emitted from turbofan aircraft engines is an ongoing challenge. For continued progress, it is necessary to assess the performance of the most recent prediction methods in the NASA Aircraft NOise Prediction Program (ANOPP), and to examine the effects of flight condition on fan noise. The assessment is based on an extensive acoustic dataset acquired as part of the Propulsion Airframe Aeroacoustics and Aircraft System Noise (PAA&ASN) Flight Test conducted on a Boeing 787-10 aircraft. Engine operating condition was varied to study the characteristics of fan noise in flight. In a subset of the flight test matrix, the influence of the aft duct acoustic liner was studied by covering the lined area with aluminum tape to simulate a hardwall duct. The combination of test data at different flight conditions, along with rigorous predictions of jet noise, is used in this paper to extract fan noise from the measured total aircraft noise levels. The measured fan noise levels are compared with those predicted using the latest methods for fan source noise, liner attenuation, and PAA effect prediction. Detailed analyses are undertaken to understand agreement between data and various aspects of the prediction models, including spectral shape, directivity, and response to throttle setting. An additional investigation was undertaken to study the effect of aircraft speed on fan noise, as current models do not directly account for this parameter.

Aircraft System Noise↗

NASA NTRSDate not supplied

Quantification of Numerical Uncertainty via Nonlinear Dynamical Approach

Motivations (Ensure a Higher Level of Confidence in the Predictability & Reliability of Numerical Simulation for Multiscale Complex Nonlinear Fluid Problems) - The last two decades have been an era when computation is ahead of analysis & when very large scale practical computations are increasingly used in poorly understood multiscale complex nonlinear physical problems & non-traditional fields (Especially when computations offer the ONLY way of generating this type of data limited simulations). - At present some of the numerical uncertainties can be explained and minimized by traditional numerical analysis and standard CFD practices. However, such practices, usually based on linearized analysis, MIGHT NOT be sufficient for strongly nonlinear and/or stiff problems. - We need a good understanding of the nonlinear behavior of numerical schemes being used as an integral part of code verification, validation and certification.

HEC↗

NASA NTRSDate not supplied

Validation of A Simulation Environment for Future Space Traffic Management

This study presents initial results of a newly developed simulation environment intendedto explore and assess future Space Traffic Management (STM) scenarios. The number ofnew Resident Space Objects (RSOs) in near-Earth orbit is expected to increase significantlywith the expected future deployment of a number of large constellations. These futurescenarios involve the addition of many tens of thousands of new RSOs, making the analysisinto their impact on collision risk extend beyond what traditional data-mining of present-dayconjunction data can reliably predict. To address this, a robust simulation environment wasdeveloped that implements a full force-model for orbit propagation, and computes continuousall-on-all conjunction statistics for arbitrarily large catalog sizes and simulation timeframes.Collision avoidance and station-keeping maneuvers can be optionally implemented based onconfigurable user inputs including physical characteristics and spacecraft meta-data (e.g.,commercial/government, owner country, etc.). Constellation build-out and de-orbit scenarioswere also implemented and modeled based on real-data analysis. Validation of the simulationresults was a critical component of the simulation development, and was done using the currentcatalog with comparisons against both public and internal NASA data-sets. The comparisonsdemonstrate that, with the appropriate settings, representative levels of conjunction ratesand probabilities can be obtained, providing confidence that the simulation tool can generatemeaningful outcomes for test scenarios. As an initial demonstration of the tool’s capabilities,year-long simulations with station-keeping were conducted to examine conjunction historiesusing both the current object catalog (5800 active satellites) and a hypothetical 60,000 objectscenario involving five potential large constellations. Output metrics include the number ofconjunction events, estimates of collision consequence (fragmentation), delta-V maneuver costs,and the probability of at least one collision occurring. The results highlight the potential thatthe simulation tool has for incorporating and running performance comparisons between, e.g.,various sets of maneuver guidelines, industry norms, and definitions of risk, with the overallobjective of providing actionable data to STM policy makers. The presentation will providean overview of the simulation development and validation efforts, as well as a discussion ofobservations gathered from the initial simulations performed.

conjunction assessment↗

NASA NTRSDate not supplied

Wall-Modeled Large-Eddy Simulation of Supersonic Parachute Inflation

Supersonic parachutes have been used in nearly every robotic mission to another planetary body with an atmosphere because they are one of the most mass-efficient ways to decelerate a payload to land on the surface. Short of performing flight tests in the upper Earth atmosphere, we currently cannot reliably predict a novel parachute system’s performance or potential failure modes, or even confidently explain it after the fact, as was the case with the Low Density Supersonic Decelerator flight tests and subsequent investigations. Fluid-structure interaction (FSI) simulations have the potential to bridge this gap. To this end, we present several improvements to the state-of-the-art for simulating supersonic parachutes using FSI: a higher effective resolution convective flux, an immersed boundary turbulent wall layer modeling approach to capture viscous effects, and a novel method to obtain a more realistic initial parachute shape. A recent supersonic parachute flight test is simulated and compared to measurements for the purposes of model validation.

ESM↗

NASA NTRS2025

Modeling and Simulation Credibility Assessments of Musculoskeletal Computational Models for Simulating Astronaut Injuries Due to a Poor Spacesuit Fit

The musculoskeletal (MS) system of astronauts is subject to physiological changes, potentially leading to injuries due to the exposure to different gravitational environments experienced during spaceflight. These injuries can occur while an astronaut is performing an Extravehicular Activity (EVA) in space, on lunar or planetary surfaces or while wearing a spacesuit during terrestrial training for an EVA. The OpenSim MS modeling software can assess EVA induced MS injury mechanisms such as muscle strains, ligament injuries and joint injuries. One area of concern, since there are only a few different spacesuit sizes with limited adjustability, is the possibility of a poorly fitting spacesuit. This can cause unnatural joint motions and torques resulting in various MS injuries. A credibility assessment of the OpenSim modeling and simulation procedures is performed per NASA-STD-7009A to provide information on the credibility of the model’s use in simulating EVA related injury mechanisms. The credibility assessment evaluated various OpenSim models against the following eight credibility factors: data pedigree, input pedigree, code verification, solution verification, conceptual validation, referent validation, results uncertainty and results robustness (sensitivity). The models evaluated for EVA injuries will require additional credibility factor analysis and upgrades to the model features, such as adding ligaments to a whole-body model, to reliably predict and analyze the EVA injuries expected to occur due to a poor spacesuit fit. The degree of elevation strategy required to increase the credibility assessment scores will depend on the model complexity and the injury mechanism.

Christopher A. Gallo↗

NASA NTRS2025

Model-Based Engineering/Digital Engineering (MBE/DE) and Mission Assurance of Complex NASA Systems With Federated Modeling

Explore the source record for details and available documents.

systems engineering↗

NASA NTRS2024

Modeling and Simulation Credibility Assessments of Musculoskeletal Computational Models for Simulating Astronaut Injuries Due to a Poor Spacesuit Fit

Christopher A Gallo↗

NASA NTRS2023

Satellite characterization of global stratospheric sulfate aerosols released by Tonga volcano

Large volcanic eruptions create an enhanced layer of sulfate aerosols in the stratosphere. These sulfuric acid droplets persist for many months, altering the climate and stratospheric chemistry. Sulfate aerosols scatter sunlight back to space, cooling the surface of the Earth and absorb outgoing thermal radiation, heating the stratosphere. The calculation of the climate impact of sulfate aerosols depends on their physical properties such as droplet size and chemical composition. These properties are not well known, and this uncertainty contributes to the errors in climate model predictions. Here we derive the first empirical formula that predicts the composition of stratospheric sulfate aerosols from volcanic eruptions from the air temperature and water vapor pressure. Measurements of atmospheric infrared transmittance of the Hunga Tonga-Hunga Ha'apai sulfate aerosol plume by the Atmospheric Chemistry Experiment (ACE) satellite were analyzed to determine composition (weight percent of sulfuric acid) and median particle radius. These data are supplemented by measurements of the Raikoke and Nabro eruptions. Our analysis allows the properties of volcanic aerosols in the stratosphere to be predicted reliably in atmospheric models.

P Bernath↗

DOE OSTI2024

Statistical and Neural Network for Real Sensor-Data-Driven Anomaly Detection in Nuclear Applications

Anomaly detection (AD) in sensor data is critical to ensure uninterrupted functionality of nuclear power plants (NPPs). Consequently, AD model validation through real-world sensor data is important for applications in nuclear facilities. In this paper, we propose an Autoencoder (AE)—a multi-layered neural network, for AD in sensor data from an operational NPP testbed. Since the dataset lacks labels for irregularities, we introduce random noise and label them to effectively train our model. The proposed AE model assigns a higher reconstruction error to the abnormal samples that deviate from those encountered during the training phase and uses the reconstruction loss to detect anomalies in a representative imbalanced dataset. We also introduce an analytical solution—seasonal trend decomposition (STD)—as another AD scheme for identifying irregularities withinthe same time-series dataset. In contrast to the AE model which relies on reconstruction loss, the STD scheme decomposes the entire dataset into its trend, seasonality, and residual components to pinpoint irregularities. Our findings indicate that the proposed AE and STD models individually achieve recall scores of 97% and 92%, respectively. We validate the performance of the two models on both balanced and imbalanced data. We further solidify the results by picking the combined selected anomalies of the two solutions with an "AND" operator for more reliable predictions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Statistical and Neural Network for Real Sensor-Data-Driven Anomaly Detection in Nuclear Applications

Anomaly detection (AD) in sensor data is critical to ensure uninterrupted functionality of nuclear power plants (NPPs). Consequently, validation of AD models through real-world sensor data is important for their application in nuclear facilities. In this paper, we propose an Autoencoder (AE)— a multi-layered neural network, for AD in sensor data from an operational NPP testbed. Since the dataset lacks labels for irregularities, we introduce random noise and label them to effectively train our model. The proposed AE model assigns a higher reconstruction error to the abnormal samples that deviate from those encountered during the training phase and uses the reconstruction loss to detect anomalies in a representative imbalanced dataset. We also introduce an analytical solution—seasonal trend decomposition (STD) — as another AD scheme for identifying irregularities within the same time-series dataset. In contrast to the AE model which relies on reconstruction loss, the STD scheme decomposes the entire dataset into its trend, seasonality, and residual components to pinpoint irregularities. Our findings indicate that the proposed AE and STD models individually achieve recall scores of 97% and 92%, respectively. We also validate the performance of the two models on both balanced and imbalanced data. We further solidify the results by picking the combined selected anomalies of the two solutions with an "AND" operator for more reliable predictions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Colloidal Behavior of Plutonium Oxide in Concentrated Electrolyte Solutions

The Hanford Site in Washington State manages legacy high-level radioactive waste streams that display major chemistry and engineering challenges, including the high salt levels and pH values that correspond to conditions under which many classical concepts describing chemical reactivity cannot be applied. One particular challenge that needs to be tackled at Hanford is that Pu concentrations, [Pu], in the soluble phases of the tank wastes are higher than expected based on the solubility of crystalline PuO2, which is widely accepted to be caused by the formation of PuO2 colloid, consisting of nano- to submicron-sized particles (PuO2 NPs). Fundamental research underpinning the behavior of PuO2 NPs under conditions not only relevant to the Hanford tank waste but at high ionic strength in general is needed to reliably predict the chemical reactivity of PuO2 NPs and develop engineering solutions to safely and efficiently process high-level radioactive waste into forms suitable for long-term storage. In this work, we study the behavior of PuO2 NPs (particle size ~100 nm) under high ionic strength conditions by reacting it with highly concentrated (up to 5 M) salt solutions. We explore different electrolyte compositions to elucidate the impact of different anions (NO3-, Cl-, ClO4-, SO42-, C2O42-, CO32-) on the stability of PuO2 NP in the acidic and alkaline pH regime. PuO2 NP aggregation and precipitation as function electrolyte concentration is tracked by a combination of liquid scintillation counting, dynamic light scattering for determination of particle size distributions, and zeta potentials as a proxy for particle charge. At acidic pH, electrolytes containing non-coordinating anions, such as NaNO3, NaCl, and NaClO4 mostly stabilize PuO2 NPs over a large electrolyte concentration range, showing only subtle differences in their reactivity. Other electrolyte anions show a more pronounced effect on the PuO2 NP stability: SO42-, binds directly to the particles’ surface, reverses the particle charge, and precipitates the PuO2 NPs efficiently even at intermediate sulfate concentrations (>0.1 M). In contrast, C2O42- is found to lead to high [Pu] in solution, in the milli-molar range, even at mildly acidic pH (~4). Thermodynamic modeling of the dissolved Pu concentrations using PHREEQC is unable to predict the observed [Pu] in the acidic pH regime, supporting the influence of colloids in maintaining elevated [Pu]. It is noteworthy that the current thermodynamic databases do not include constants for colloidal Pu phases and cannot accurately predict many of the high ionic strength solutions relevant to this work. The mechanisms and models responsible for these observations will need further investigation in the future. At high pH values (~12), PuO2 NPs exhibits classical sol-gel chemistry, meaning that upon destabilization of the colloidal sol, for example by addition of concentrated NaOH, highly porous and viscid PuO2 coagulates are formed that consist of a three-dimensional network likely held together by physical interactions. The PuO2 NP coagulate shows no significant reversibility of the aggregation when contacted with concentrated brines; however, PuO2 NPs can be efficiently resuspended in solution by addition of diluted electrolytes, alkaline solutions containing high amounts of carbonate, or simple addition of water. Especially carbonate is shown to stabilize PuO2 NPs in solution at high pH, characterized by stable colloidal suspensions that are resistant against sedimentation during centrifugation. Thermodynamic modeling of the carbonate system was able to predict an increasing dissolved Pu concentration with increasing carbonate concentration. However, the model was profoundly sensitive to the fixed redox potential and does not include any thermodynamic constants for colloidal Pu species.

Neumann, Julia↗