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DOE OSTI2023

Modeling Geologic Waste Repository Systems Below Residual Saturation

The heat generated by high-level radioactive waste can pose numerical and physical challenges to subsurface flow and transport simulators if the liquid water content in a region near the waste package approaches residual saturation due to evaporation. Here, residual saturation is the fraction of the pore space occupied by liquid water when the hydraulic connectivity through a porous medium is lost, preventing the flow of liquid water. While conventional capillary pressure models represent residual saturation using asymptotically large values of capillary pressure, here, residual saturation is effectively modeled as a tortuosity effect alone. Treating the residual fluid as primarily dead-end pores and adsorbed films, relative permeability is independent of capillary pressure below residual saturation. To test this approach, PFLOTRAN is then used to simulate thermal-hydrological conditions resulting from direct disposal of a dual-purpose canister in unsaturated alluvium using both conventional asymptotic and revised, smooth models. Importantly, while the two models have comparable results over 100 000 years, the number of flow steps required is reduced by approximately 94%.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Vitrification of Hanford Tank 241-AP-101 Waste and Simulant

Hanford tank 241-AP-101 (referred to herein as AP-101) is the second Hanford radioactive tank waste planned to be processed and vitrified. A simulant version of AP 101 waste was formulated from the best-basis inventory (BBI) for the Hanford Tank 241-AP-101 liquid with an assumed target dilution of the waste from the BBI sodium molarity of 8.61 M to the desired 5.5 M Na. After the addition of glass-forming chemicals (GFCs), the simulant melter feed was processed in a non-radioactive, continuous laboratory-scale melter (CLSM) system. The AP-101 simulant melter feed was charged into the CLSM for 6.11 h of processing, which produced 6.55 kg of glass, for an average glass production rate of 2275 kg m 2 d -1 . Since there were no processing issues with the AP-101 simulant melter feed, AP-101 melter feed made with actual waste was then processed in a CLSM system built into a contamination area in a radioactive environment. The melting behavior characteristics appeared similar for both the simulant and waste melter feeds. The AP-101 waste melter feed was charged into the CLSM for 12.14 h of processing, which produced 8.75 kg of glass, for an average glass production rate of 1530 kg m 2 d -1 . During the AP-101 waste melter feed charging, the pump used to move the feed reached a maximum and it is believed that if the pump had a greater capacity, a greater average glass production rate could have been achieved. A constituent of interest present in low quantities in the AP-101 waste is 99 Tc or its non-radioactive surrogate, Re, added to the AP-101 simulant. Analysis for the quantities of 99 Tc and Re in the AP-101 glass product resulted in an average single-pass retention from the melter feed during relative chemical steady state of 55 ± 2 % for 99 Tc and 45 ± 2 % for Re. Compared to the processing of other melter feeds, the retention of 99 Tc in the AP-101 glass was greater than in both AP-107 and AP-105 glass, while the retention of Re in the AP-101 was less than in the AP-107 glass, but greater than in the AP-105 glass. A spike of I was added into the AP-101 melter feed that could be detected above the analysis detection limits. However, the iodine was only detectable above the ~6 ppm limit in one glass pour: the pour immediately following the burn off of the cold cap, where the I level reached ~30 ppm. This event was significant because the glass was poured immediately after burn off and thus it is presumed that the iodine had yet to volatilize from the glass melt while idling. It is recommended to perform future tests with I spikes at greater levels so that it can be detected in additional glass pours to determine if the expected 50 % retention of I used in the Kim et al. glass models can be confirmed. Offgas liquid samples were analyzed for acetonitrile, which was present at greater concentrations in CLSM liquids than in other scaled melter systems. This result was expected based on unique conditions with the CLSM system including a small plenum space leading to low residence time for offgas and the rapidity of offgas cooling upon exiting the CLSM vessel due to the location and environment. About 90 % of the total acetonitrile captured during both the AP-101 simulant and waste CLSM runs was found in the offgas condensate and demister liquids, thus it is recommended that only those liquids be sent for analysis if future testing to study the presence of acetonitrile in offgas products is desired.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Kinetics of the Temperature-Dependent e aq - and ·OH Radical Reactions with Cr(III) Ions in Aqueous Solutions

The reactivity of chromium(III) species with the major oxidizing and reducing radiolysis products of water was investigated in aqueous solutions at temperatures up to 150 °C. The reaction between the hydrated electron (e aq - ) and Cr(III) species showed a positive temperature dependence over this temperature range. The reaction was also studied in pH 2.5 and 3.5 solutions for the first time. This work also studied the reaction between acidic Cr(III) species and the hydroxyl radical (·OH). It was found that Cr 3+ did not react significantly with the ·OH radical, but the first hydrolysis species, Cr(OH) 2+ , did with a rate coefficient of k= (7.2±0.3)×10 8 M -1 s -1 at 25 °C. The oxidation of Cr(OH) 2+ by the ·OH radical formed an absorbing product species that ultimately oxidized to give Cr(VI). In conclusion, these newly measured reaction rates allow for the development of improved models of aqueous chromium speciation for the effective remediation of liquid high-level nuclear waste via vitrification processes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

Transport Cost for Carbon Removal Projects With Biomass and CO2 Storage

Strategies to remove carbon from the atmosphere are needed to meet global climate goals. Promising strategies include the conversion of waste biomass to hydrogen, methane, liquid fuels, or electricity coupled with CO 2 capture and storage (CCS). A key challenge for these projects is the need to connect geographically dispersed biomass supplies with geologic storage sites by either transporting biomass or CO 2 . We assess the cost of transport for biomass conversion projects with CCS using publicly available cost data for trucking, rail, and CO 2 pipelines in the United States. We find that for large projects (order of 1 Mt/yr CO 2 or greater), CO 2 by pipeline is the lowest cost option. However, for projects that send most of the biomass carbon to storage, such as gasification to hydrogen or electricity production, biomass by rail is a competitive option. For smaller projects and lower fractions of carbon sent to storage, such as for pyrolysis to liquid fuels, CO 2 by rail is the lowest cost option. Assessing three plausible example projects in the United States, we estimate that total transport costs range from $24/t-CO 2 stored for a gasification to hydrogen project traversing 670 km to $\$ 36$/t for a gasification to renewable natural gas project traversing 530 km. In general, if developers have flexibility in choosing transport mode and project type, biomass sources and storage sites can be connected across hundreds of kilometers for transport costs in the range of $20-40/t-CO 2 stored. Truck and rail are often viable modes when pipelines cannot be constructed. Distances of 1,000 km or more can be connected in the same cost range when shared CO 2 pipelines are employed.

09 BIOMASS FUELS↗

NASA NTRS1924

Combustion of liquid fuels in diesel engine

Hitherto, definite specifications have always been made for fuel oils and they have been classified as more or less good or non-utilizable. The present aim, however, is to build Diesel engines capable of using even the poorest liquid fuels and especially the waste products of the oil industry, without special chemical or physical preparation.

FUELS↗

DOE OSTI2022

Impact of Variable Gas Mixtures on Bubble Size Distribution and Mass Transfer in Gas Fermentation Reactors

Gas fermentation has emerged as a promising new technology for the generation of fuels and chemicals from mixtures of greenhouse and energy rich gas streams (CO2/CH4/H2/CO) via microbial bioreaction. Example pathways include biomethanation (CO2/H2 to CH4), biogas upgrading, CO fermentation and wet-waste conversion. Effective Gas-liquid mass-transfer is an important physical phenomenon that determines the design and scale-up of these systems. There is currently a knowledge-gap regarding bubble-size distributions when using a mixture of gases with vastly different properties, which can have a significant impact on overall mass-transfer. For example, hydrogen bubbles are more buoyant compared to other relatively heavier gases (CO2/CH4/CO), resulting in a large distribution of residence times and bubble sizes. This work therefore develops a deeper understanding of bubble dynamics and interphase mass transfer in such heterogenous gas mixtures through well-resolved computational models. We use a detailed multiphase computational-fluid-dynamics (CFD) model to study the impact of gas-mixtures on overall mass-transfer in bubble column and air-lift reactors. The CFD tool previously developed by the authors (1) for simulating aerobic fermentation reactors at scale is used in this study. The Reynolds-averaged mass, momentum, energy, and species transport equations are solved for interpenetrating gas and liquid phase in this model. We use a population balance-based bubble-size-distribution model that is validated against small-scale experiments in our solver. Results pertaining to multiple simulations of gas-fermentation reactors are presented where gas mixtures with varying compositions of CO2/CH4/CO/H2 are imposed at the sparger boundaries. The spatio-temporal variations in bubble-size distribution and mass transfer coefficient is analyzed for varying superficial velocities and gas-compositions for varying sizes of bubble-column and airlift reactors.

BIOMASS FUELS,MATHEMATICS AND COMPUTING↗

DOE OSTI2022

Quantifying Antibiotic Distribution in Solid and Liquid Fractions of Manure Using a Two-Step, Multi-Residue Antibiotic Extraction

Antibiotic distribution and analysis within liquid and solid fractions of manure are highly variable due to each compound’s respective physiochemical properties. This study developed and evaluated a uniform method extracting 10 antibiotics from 4 antibiotic classes (tetracycline, sulfonamides, macrolides, and β-lactam) from unprocessed manure, solid–liquid separated manure, and composted solids. Through systematic manipulation of previously published liquid chromatography tandem mass spectrometry methods; this study developed an extraction protocol with optimized recovery efficiencies for varied manure substrates. The method includes a two-step, liquid-solid extraction using 10 mL of 0.1 M EDTA-McIlviane buffer followed by 10 mL of methanol. Antibiotics recoveries from unprocessed manure, separated liquids, separated solids, and heat-treated solids using the two-step extraction method had relative standard deviations < 30% for all but ceftiofur. Total antibiotic recoveries were 67–131% for tetracyclines, 56% for sulfonamide, 49–53% for macrolides, and 1.3–66% for β-lactams. This is the first study to use one protocol to assess four classes of antibiotics in liquid and solid manure fractions. This study allowed for more precise risk assessment of antibiotic transport in manure waste stream applied to fields as a liquid or solid compost.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Demonstrating the Feasibility of Biomass Pyrolysis Liquid, Coal, Plastic Oil Mixtures for Entrained Flow Gasification

There is interest in co-gasifying coal, biomass and plastic. An attractive alternative is to do that in a pressurized entrained-flow gasifier, technology that has been used for coal gasification for decades. The approach taken in this study is to liquefy biomass through fast pyrolysis and to liquefy waste plastic by thermal decomposition. The liquids form the basis of a slurry that also includes coal particles. In this work, several different compositions of coal-bioliquid-plastic oil slurries were prepared and evaluated for viscosity and settling properties. Suitable composition ranges were identified and are highlighted in the presentation.

Hughey, Logan↗

NASA NTRS1978

Simultaneous treatment of SO2 containing stack gases and waste water

A process for simultaneously removing sulfur dioxide from stack gases and the like and purifying waste water such as derived from domestic sewage is described. A portion of the gas stream and a portion of the waste water, the latter containing dissolved iron and having an acidic pH, are contacted in a closed loop gas-liquid scrubbing zone to effect absorption of the sulfur dioxide into the waste water. A second portion of the gas stream and a second portion of the waste water are controlled in an open loop gas-liquid scrubbing zone. The second portion of the waste water contains a lesser amount of iron than the first portion of the waste water. Contacting in the openloop scrubbing zone is sufficient to acidify the waste water which is then treated to remove solids originally present.

Poradek, J. C.↗

DOE OSTI2024

Development of a Liquid Bridge Model for Particle Agglomeration and Defluidization in Plastic Pyrolysis

Molten plastic that forms during the pyrolysis of plastic or municipal solid waste feedstock can lead to particle agglomeration. A liquid bridge model is developed in MFiX-DEM and validated against a cold flow experiment with glass beads coated with silicone oil. The liquid bridge model is then extended to support an evolving liquid layer thickness for pyrolysis applications. The extended model is used to study the sensitivity of the pyrolysis reactor to solids holdup, flow conditions, and plastic properties.

Banerjee, Subhodeep↗

DOE OSTI2020

Solubility Predictions for Hanford Tank Concentrates with HSC - 20459

The commercially available Outotec HSC 9.9.0{sup R} provides excellent predictions for the solubilities of many species for Hanford waste tank concentrates. The HSC solubility predictions with a Harvie activity model agreed well with five boildowns that showed solubility limits for NaNO{sub 3}, NaNO{sub 2}, Na{sub 2}CO{sub 3}, NaF, Na{sub 2}SO{sub 4}, and Na{sub 3}PO{sub 4}. However, the HSC did not predict density and therefore water content very well and therefore we used the measured densities and derived water content from the difference between measured density and assays. Furthermore, we adjusted the HSC enthalpy for the minor species Na{sub 3}PO{sub 4}*NaF double salt in order to fit the five boildowns as well. Previous work has shown that gibbsite becomes and remains supersaturated in all of these boildowns and so there was no alumina precipitation despite supersaturation. Furthermore, an equilibrium model like HSC always shows complete oxidation of any TOC in the presence of nitrate and nitrite. We therefore suppressed the HSC oxidation of acetate and oxalate in order to fit measured acetate and oxalate solubilities as TOC. Space in Hanford waste tanks is very limited and therefore evaporator campaigns continue to recover needed tank space from dilute tank liquids. Prior to each evaporator campaign, a boildown of a sample of tank liquid for each campaign provides a basis for planning by measuring density, water activity, soluble species, and solids precipitation as a function of concentration at 18 deg. C. These boildowns then provide validations and calibrations for the HSC solubility prediction for Hanford wastes. Previous work has shown the solubilities of minor electrolytes in these five boildowns follow rather simple power law solubility products. Hanford's 222-S laboratory has reported each of five boildowns for concentrated liquids from five waste tanks and tank blends. All boildowns eventually showed the precipitation of the dominant electrolyte, NaNO{sub 3}, and overall solution activity largely drives all solubility. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS2003

Lyophilization for Water Recovery From Solid Waste

This abstract describes the development of a solid waste treatment system designed for a near term human exploration mission. The technology being developed is an energy- efficient lyophilization technique that recovers water from spacecraft solid waste. In the lyophilization process water in an aqueous waste is frozen and then sublimed, resulting in the separation of the waste into a dried solid material and liquid water. This technology is ideally suited to applications where water recovery rates approaching 100% are desirable but production of CO, is not. Water contained within solid wastes accounts for approximately 3% of the total water balance. If 100% closure of the water loop is desired the water contained within this waste would need to be recovered. To facilitate operation in microgravity thermoelectric heat pumps have be used in place of traditional fluid cycle heat pumps. A mathematical model of a thermoelectric lyophilizer has been developed and used to generate energy use and processing rate parameters. The results of laboratory investigations and discussions with ALS program management have been used to iteratively arrive at a prototype design. This design address operational limitations which were identified in the laboratory studies and handling and health concerns raised by ALS program management. The current prototype design is capable of integration into the ISS Waste Collection System.

Flynn, Michael↗

NASA NTRS1995

Prototype development and test results of a continuous ambient air monitoring system for hydrazine at the 10 ppb level

A Hydrazine Vapor Area Monitor (HVAM) system is currently being field tested as a detector for the presence of hydrazine in ambient air. The MDA/Polymetron Hydrazine Analyzer has been incorporated within the HVAM system as the core detector. This analyzer is a three-electrode liquid analyzer typically used in boiler feed water applications. The HVAM system incorporates a dual-phase sample collection/transport method which simultaneously pulls ambient air samples containing hydrazine and a very dilute sulfuric acid solution (0.0001 M) down a length of 1/4 inch outside diameter (OD) tubing from a remote site to the analyzer. The hydrazine-laden dilute acid stream is separated from the air and the pH is adjusted by addition of a dilute caustic solution to a pH greater than 10.2 prior to analysis. Both the dilute acid and caustic used by the HVAM are continuously generated during system operation on an "as needed" basis by mixing a metered amount of concentrated acid/base with dilution water. All of the waste water generated by the analyzer is purified for reuse by Barnstead ion-exchange cartridges so that the entire system minimizes the generation of waste materials. The pumping of all liquid streams and mixing of the caustic solution and dilution water with the incoming sample are done by a single pump motor fitted with the appropriate mix of peristaltic pump heads. The signal to noise (S/N) ratio of the analyzer has been enhanced by adding a stirrer in the MDA liquid cell to provide mixing normally generated by the high liquid flow rate designed by the manufacturer. An onboard microprocessor continuously monitors liquid levels, sample vacuum, and liquid leak sensors, as well as handles communications and other system functions (such as shut down should system malfunctions or errors occur). The overall system response of the HVAM can be automatically checked at regular intervals by measuring the analyzer response to a metered amount of calibration standard injected into the dilute acid stream. The HVAM system provides two measurement ranges (threshold limit value (TLV): 10 to 1000 parts per billion (ppb)/LEAK: 100 ppb to 10 parts per million (ppm)). The LEAK range is created by dilution of the sulfuric acid/hydrazine liquid sample with pure water. This dual range capability permits the analyzer to quantify ambient air samples whose hydrazine concentrations range from 10 ppb to as high as 10 ppm. The laboratory and field prototypes have demonstrated total system response times on the order of 10 to 12 minutes for samples ranging from 10 to 900 ppb in the lLV mode and is greater than 2 minutes for samples ranging from 100 to 1300 ppb in the LEAK mode. Service intervals of over 3 months have been demonstrated for continuous 24 hour/day, 7 day/week usage. The HVAM is made up of a purged cabinet that contains power supplies, RS422 signal transmission capabilities, a UPS, an on-site warning system, and a Line Replaceable Unit (LRU). The LRU includes all of the liquid flow system, the analyzer, the control/data system microprocessor and assorted flow and liquid-level sensors. The LRU is mounted on a track slide system so it can be serviced inplace or totally removed and quickly exchanged with another calibrated unit, thus minimizing analyzer downtime. Once an LRU is removed from an analyzer enclosure, it can be brought to a laboratory facility for complete calibration and periodic maintenance.

Meneghelli, Barry↗

DOE OSTI2023

Near-Critical CO 2 -Assisted Liquefaction-Extraction of Biomass and Wastes to Fuels and Value-Added Products

With the growing need for sustainable carbon-neutral liquid fuels, low-grade feedstocks, such as lignocellulosic biomass, and municipal solid wastes offer sufficient potential via thermochemical conversion. But the existing thermochemical means are limited in feed flexibility and scalability and require significant processing (energy and costs) of the intermediates. Bio-oil/biocrude intermediate from fast pyrolysis and hydrothermal techniques is impeded by issues of stability and oxygen content, along with hydrotreating viability. To address these issues, we investigated a novel pathway of near-critical CO 2 -assisted integrated liquefaction-extraction (NILE) technology in conceptual aspects for conversion of various biomass and municipal solid wastes into high-quality biocrude with high compatibility for co-hydrotreating with traditional fossil crude for liquid fuel needs in power and transportation sectors. Using supercritical CO 2 for dewatering wet feedstocks, for liquefaction, and extraction for lighter biocrude has produced biocrude with lower oxygen content by 50%, lowered metal content by 90%, stable viscosity, low acidity, and good aging stability compared to that produced from hydrothermal liquefaction along with higher hydrotreating and co-hydrotreating compatibility. Hydrotreating of the biocrude extract from supercritical CO 2 extraction also was feasible with no detected coke deposition, an oxygen content of 1%, and catalyst deactivation. Here, the validation and capabilities of the NILE concept urge for its further development to obtain sustainable liquid fuels with lower greenhouse gas emissions and costs.

09 BIOMASS FUELS↗

DOE OSTI2021

An Evaluation of the Impact of Glycolate and Glycolate Mitigation on the Defense Waste Processing Facility Recycle Diversion Project Flowsheet

The Savannah River Site (SRS) Defense Waste Processing Facility (DWPF) processes radioactive High Level Waste (HLW) sludge solids from the Concentration, Storage, and Transfer Facilities (CSTF); which includes the SRS Tank Farm and Evaporator facilities, and a concentrated Cs-137 laden stream and a Monosodium Titanate (MST) and sludge solids stream from the SRS Salt Waste Processing Facility (SWPF). The waste is chemically adjusted with acids and reductant (currently with 50 wt.% nitric acid and ~90 wt.% formic acid, but eventually formic acid will be substituted with ~70 wt.% glycolic acid), and frit is added so that a durable, borosilicate glass waste form can be produced when the material is vitrified in the melter. As a result of the evaporation of water during both the melter feed preparation and the melter feed vitrification steps in DWPF, a recycle waste stream is generated, neutralized, and sent back to the CSTF. The recycle waste is a dilute aqueous stream originating from the collection of condensate liquids containing some minor sludge, MST, and frit solids and other waste components resulting from melter feed entrainment during foamover events and transfer of volatile species into the condensate. The recycle stream volume is significant and is expected to approach 3 million gallons per year once SWPF reaches full operation, requiring the use of multiple large CSTF tanks for storage. The recycle waste is currently collected in the SRS Tank Farm and periodically evaporated in the 242-16H (2H) Evaporator to conserve storage space.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS2024

Rapid Composting of Crop Space Waste

This project processed multiple types of waste simulant feedstocks using commercial composting units and NASA Trash-to-Gas (TtG) technology processing units to see what solids, liquids, and gases could be recovered. The feedstock waste included inedible biomass, mission waste from the Johnson Space Center (JSC) Crew Health and Performance Exploration Analog (CHAPEA), Mars analog, and the long duration Orbital Syngas/Commodity Augmentation Reactor (OSCAR) Waste Simulant (OWS) and OSCAR Full Scale (FS) (also referred to as Mars 850-day mission waste simulant). The performance data was collected, and overall performance of the waste processing systems, as well as elemental analysis of the product yields for enabling Lunar and Martian regolith mixtures in a crop grow-out study, were performed. Germination took place in certain Lunar and Martian regolith studies, with promising preliminary results that TtG solid products can be used as plant nutrients to enable crop growth in off-world regolith simulants.

Anne Meier↗

NASA NTRS1984

The Liquid Droplet Radiator - an Ultralightweight Heat Rejection System for Efficient Energy Conversion in Space

A heat rejection system for space is described which uses a recirculating free stream of liquid droplets in place of a solid surface to radiate waste heat. By using sufficiently small droplets ( 100 micron diameter) of low vapor pressure liquids the radiating droplet sheet can be made many times lighter than the lightest solid surface radiators (heat pipes). The liquid droplet radiator (LDR) is less vulnerable to damage by micrometeoroids than solid surface radiators, and may be transported into space far more efficiently. Analyses are presented of LDR applications in thermal and photovoltaic energy conversion which indicate that fluid handling components (droplet generator, droplet collector, heat exchanger, and pump) may comprise most of the radiator system mass. Even the unoptimized models employed yield LDR system masses less than heat pipe radiator system masses, and significant improvement is expected using design approaches that incorporate fluid handling components more efficiently. Technical problems (e.g., spacecraft contamination and electrostatic deflection of droplets) unique to this method of heat rejectioon are discussed and solutions are suggested.

A T Mattick↗

DOE OSTI2022

Model Validation for the FY2021 SRS Composite Analysis Monitoring Plan

Using a projected end-state date of 2065 (SRNS 2015b), the Savannah River Site (SRS) Composite Analysis (CA) modeling for each facility and waste site began on the inventory year assigned to it so that source depletion and radionuclide transport out of the system could be appropriately captured. Some SRS waste sites that have already achieved their end states (i.e., end-state inventories and end-state configuration) are currently contributing to the potential off-site public dose through source release, groundwater transport, discharge to on-site surface streams, and stream transport to the CA point of assessments (POAs). The inventory year assigned to these waste sites is 2002 or before. This means that SRS CA results from 2002 and beyond are a reasonable representation for these waste sites that have already achieved their end states and are currently contributing to the potential off-site public dose. The SRS Annual Environmental Report (AER) monitoring can differentiate and separate liquid pathway data allowing the data representing only waste sites at their end state to be produced. Because the SRS CA has projected reasonable end-state impacts from 2002 and beyond, and the AER monitoring can differentiate and separate operating and end-state contributions to annual liquid pathway release, an opportunity exists to use the AER monitoring data to validate the SRS CA model.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗