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At least 685 records · Page 38

Organic Acid-Assisted Thermal Dehalogenation of Halide Salt Nuclear Wastes: From Waste Salts to Borosilicate Glass

Only a handful of high-halide salt waste forms have been demonstrated for vitrification-based immobilization strategies for halide-salt nuclear waste streams (e.g., pyroprocessing wastes, molten salt reactor wastes) and they all have low waste loading potential and most have low chemical durabilities for high-alkali streams. An alternative approach to direct salt immobilization is salt partitioning prior to waste form fabrication and one option for partitioning is halide removal (called dehalogenation). Removing the halogen fraction through dehalogenation can significantly reduce the waste volume required for disposal in the primary waste form. Furthermore, when dehalogenation is performed using organic acids, the dehalogenation reagent can decompose during high-temperature vitrification, reducing waste loading limitations in the waste form. In the current work, different organic acids (i.e., oxalic, formic, acetic, oxamic, and citric) were evaluated for dehalogenation efficiency of a simple chloride salt simulant (7.19% LaCl 3 , 53.77% LiCl, and 39.04% KCl, by mole) and a more complex chloride salt simulant called ERV3 (electrorefiner version 3) at 150 °C–300 °C and using H + /Cl – molar ratios of 1:1, 2:1, and 3:1. Additionally, a borosilicate glass waste form called TARS (or the average of refined specifications) was formulated, produced, and characterized for dehalogenated ERV3.

Amorphous materials↗

Fast Advective Water Flow through Nanochannels in Clay Interlayers: Implications for Moisture Transport in Soils and Unconventional Oil/Gas Production

Water flow in nanometer or sub-nanometer hydrophilic channels bears special importance in diverse fields of science and engineering. However, the nature of such water flow remains elusive. In this work, we report our molecular-modeling results on water flow in a sub-nanometer clay interlayer between two montmorillonite layers. We show that a fast advective flow can be induced by evaporation at one end of the interlayer channel, that is, a large suction pressure created by evaporation (~818 MPa) is able to drive the fast water flow through the channel (~0.88 m/s for a 46 Å-long channel). Scaled up for the pressure gradient to a 2 μm particle, the velocity of water is estimated to be about 95 μm/s, indicating that water can quickly flow through a μm-sized clay particle within seconds. The prediction seems to be confirmed by our thermogravimetric analysis of bentonite hydration and dehydration processes, which indicates that water transport at the early stage of the dehydration is a fast advective process, followed by a slow diffusion process. The possible occurrence of a fast advective water flow in clay interlayers prompts us to reassess water transport in a broad set of natural and engineered systems such as clay swelling/shrinking, moisture transport in soils, water uptake by plants, water imbibition/release in unconventional hydrocarbon reservoirs, and cap rock integrity of supercritical CO 2 storage.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Assessing the deployment of solar-driven hydrogen from biomass at scale in the U.S.

Solar hydrogen from biomass gasification is a promising technology to sustainably produce hydrogen, responsibly dispose biomass waste, and reduce reliance on fossil fuels. However, its large-scale deployment faces challenges due to the geospatial misalignment between biomass resources and solar intensity, which introduces additional supply chain logistics costs. We analyze the logistics cost burden imposed by this misalignment and its impact on successful large-scale deployment of solar-driven hydrogen from biomass in the United States. We also consider associated carbon emissions and explore how the mix of deployed technologies evolves under externally imposed carbon penalties. Our findings show that while economies of scale are known to apply at the processing facility level, the reverse effect occurs at the broader systems-level, driven by logistics. Also, at current technology costs, high carbon penalties would be required to favor deployment of solar based technologies over conventional and hybrid alternatives. We further illustrate strategies and system-level changes to reduce logistics costs and enable sustainable, low-cost hydrogen for decarbonizing different industrial sectors.

Iloeje, Chukwunwike O. [Argonne National Laborator↗

Cathode regeneration and upcycling of spent LIBs: toward sustainability

‘Green ambition towards sustainability’ is one of the hot research topics of the 21st century. With the sharp steering of the energy infrastructure toward fulfilling this radical expectation, the last decade has seen a global trend toward diversified sustainable renewable energy sources (such as solar, wind, and hydroelectric power) and electrification. Lithium-ion batteries (LIBs) are playing a significant role in this energy revolution. However, with the massive scale of the production of LIBs and their eventual retirement, attention has been turned to the erratic supply of raw materials used to manufacture these batteries and their disposal. Cathode regeneration technology is likely to be an optimal solution for the disposal of waste cathodes, aimed at non-destructively repairing and straightforwardly reusing degraded cathode materials for re-manufacturing LIBs with a shortened circular process, reasonable profits, and excellent efficiency. Additionally, cathode upcycling technology, aimed at upgrading the electrochemical performance of degraded materials, can be well adapted to the upgrading of battery chemistry and show excellent flexibility and potential for transforming the LIB industry from a resource-based to a circular economy. Thus, a holistic perspective based on the complete life cycle of LIBs is encouraged, and sustainability must be at the forefront regarding battery and pack design, raw material acquisition, materials synthesis, manufacturing, operating, retiring, and recycling processes of LIBs.

25 ENERGY STORAGE↗

Assessing the Consequences of Postclosure Criticality in Spent Nuclear Fuel

The U.S. Department of Energy is funding research into studying the consequences of postclosure criticality on the performance of a generic repository by (1) identifying the features, events, and processes (FEPs) that need to be considered in such an analysis, (2) developing the tools needed to model the relevant FEPs in a postclosure performance assessment, and (3) conducting analyses both with and without the occurrence of a postclosure criticality and comparing the results. Here, this paper describes progress in this area of research and presents the results to date of analyzing the consequences of a postulated steady-state criticality in a hypothetical saturated shale repository. Preliminary results indicate that postclosure criticality would not affect repository performance.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Physical Modeling of Coupled Thermohydraulic Behavior of Compacted MX80 Bentonite during Heating

Abstract This paper describes a tank-scale test setup and experimental methodology used to investigate coupled heat transfer and water flow processes during heating of compacted MX80 bentonite to high temperatures. Specifically, a temperature of 200°C was maintained by a cylindrical heating element at the center of a compacted bentonite layer containing an array of temperature, dielectric, and relative humidity sensors. In addition to providing an evaluation of the spatiotemporal variations in temperature, relative humidity, degree of saturation, and global volume, the coupled thermohydraulic properties of the bentonite were assessed. A wetting front was initially observed to move away from the central heater, followed by a drying process until reaching thermohydraulic equilibrium. The soil–water retention curve (SWRC) of the bentonite followed a wetting scanning path before following the primary drying path exhibiting a shift in water retention with elevated temperature. Results from the tank-scale test can be used for validation of numerical simulations of drying processes in the engineered barrier system of a high-level radioactive waste geological disposal repository and confirm that a temperature-dependent hysteretic SWRC with scanning paths is required to accurately capture the bentonite response.

Engineering↗

Waste Shipments to and from the Nevada National Security Site, Radioactive Waste Management Complex (Q3 Transportation Report, FY20) Transportation Report

This report satisfies the U.S. Department of Energy, National Nuclear Security Administration Nevada Field Office (NNSA/NFO) commitment to prepare a quarterly summary of waste shipments to the Nevada National Security Site (NNSS) Radioactive Waste Management Complex (RWMC) in Area 5.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Analytical Functions for 200 West Pump-and-Treat SCADA Sensor Data

Historical operations at the U.S. Department of Energy’s Hanford Site included disposal of waste fluids to the subsurface in the 200 West Area on the Hanford Central Plateau. Subsequent infiltration of fluids has resulted in groundwater contamination with carbon tetrachloride, nitrate, uranium, technetium-99, and other contaminants. A pump-and-treat (P&T) system, with an extraction/injection well network and an aboveground treatment plant, was implemented as part of interim and final remedies in the 200 West area. The HYPATIA single-page web application (part of the SOCRATES suite) is being developed to provide access to and analysis of chemistry and treatment facility sensor data for this 200 West P&T system. For the web application, analytical algorithms were developed to perform summing, differencing, smoothing, outlier detection, change-point detection, mass flow rate, and injectivity calculations on the data. Candidate algorithms were identified and tested, with the best-performing algorithms then assembled for implementation in HYPATIA. Because HYPATIA is hosted on the Amazon Web Services (AWS) cloud computing platform, algorithms were implemented in a back-end AWS Lambda function that can be called by the HYPATIA front end. The Lambda function applies the requested data processing to specified data via functions written in R, Python, and JavaScript. Development, testing, and review of the data analysis algorithms was completed under an NQA-1 quality program. This new HYPATIA functionality will provide information to support site decisions regarding P&T system performance and optimization.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Best Practices at the End of Photovoltaic System Performance Period

Responsible and cost-effective dissolution of photovoltaic (PV) system hardware at the end of the performance period has emerged as an important business and environmental consideration. Alternatives include extending the performance period and existing contracts for power purchase, lease, and utility interconnect; refurbishing the plant by correcting any deficiencies; repowering the plant with new PV modules and inverters; or decommissioning the plant and removing all the hardware from the site. Often key decisions are made very early in the project development and might require decommissioning by some certain date after the end of a power purchase agreement. To “abandon in place” is not an alternative acceptable to landowners and regulators, so any financial prospectus should include costs associated with decommissioning, even if those costs are deferred by extending operations, refurbishment, or repowering. Decommissioning costs are driven by regulations regarding the handling and disposal of waste, with reuse and recycling of PV modules and other components preferred as a way to reduce both costs and environmental impact. Each alternative is discussed with order-of-magnitude costs, and recommendations are provided considering site-specific details of that situation, such as estimated costs to refurbish or repower, projected revenue from continued operations, and tax considerations.

14 SOLAR ENERGY↗

Soil Sampling Results for Closure of a Portion of Solid Waste Management Unit #16

The U.S. Department of Energy/National Nuclear Security Administration (DOE/ NNSA) and National Technology & Engineering Solutions of Sandia, LLC (NTESS), the management and operating contractor for Sandia National Laboratories/California (SNL/CA), has prepared this soil sampling results report for closure of a portion of Solid Waste Management Unit (SWMU) #16. The entire network of SNL/CA sanitary sewer lines, including building laterals, was identified as SWMU #16 under a Resource Conservation and Recovery Act (RCRA) Facility Assessment conducted for SNL/CA in April 1991 (DOE 1992). Along with the previous SWMU #16 investigation results (SNL/CA 2019), the results of this investigation are intended to support closure decisions by the San Francisco Bay Regional Water Quality Control Board (RWQCB), as discussed below. SNL/CA personnel completed upgrading its sanitary sewer discharge network in 2019. These upgrades included installing new sections of underground lines and decommissioning certain sections of the old piping system by capping in place. To date, several sections of the sewer line have been abandoned-in-place by capping as new sewer lines were installed or flow was rerouted to other existing lines. To formally close these abandoned sections of the sewer line, the RWQCB required that SNL/CA personnel collect soil samples to be analyzed for contaminants potentially released from the sewer lines. SNL/CA personnel hired Weiss Associates (Weiss) of Emeryville, California to prepare a sampling and analysis plan, implement the sampling plan and report the results of the investigation under Purchase Order #2166257. The Sampling and Analysis Plan for Partial Closure of Solid Waste Management Unit #16 (SAP) was submitted to the RWQCB on August 14, 2020 by Weiss on behalf of SNL/CA. The RWQCB approved the SAP on September 30, 2020 after Weiss updated the method detection limit and reporting limits for total polychlorinated biphenyls (PCBs) and individual aroclors. Soil sampling was conducted in accordance with the SAP except that fewer locations were sampled due to site constraints, as discussed below. This report presents the results of the sampling effort and documents all associated field activities including borehole clearing, soil sample collection, storage and transportation to the analytical laboratories, borehole backfilling and surface restoration, and storage of investigation-derived waste (IDW) for future profiling and disposal by SNL/CA waste management personnel.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Air Pathway Dose Modeling for the E-Area Low-Level Waste Facility

The US Department of Energy (DOE) Order 435.1 performance assessment (PA) process (USDOE 1999) prescribes a performance objective (10 mrem y -1 ) for evaluating atmospheric releases of radionuclides from DOE low-level waste (LLW) disposal facilities. The potential dose to an individual from exposure to radionuclides released into the atmosphere from LLW disposals can be estimated by application of radionuclide-specific dose-release factors (DRFs) (mrem Ci -1 ) to estimated flux rates (Ci y -1 ) at a particular time and location. In Revision 0 of this report, Lee (2006) calculated DRFs for potential atmospheric releases of 15 volatile radionuclides from seven ELLWF disposal units in support of the 2008 ELLWF PA (WSRC 2008). The mainframe version of the US Environmental Protection Agency’s (EPA) dose model CAP88 was used in the Revision 0 assessment. In Revision 1 of this report (Dixon and Minter 2017), the site-specific Savannah River National Laboratory (SRNL) atmospheric dose models MAXDOSE-SR version 2013 (Stone and Jannik 2013a) and MAXINE version 2017 (Bell 2017) were used to calculate DRFs for ten radionuclides. Revision 2 provided updated DRFs using the current version of the US Environmental Protection Agency’s (EPA) dose model CAP88-PC Version 4.1. After Revision 2 was finalized, DRFs were requested for Ar-37, Ar-39, Kr-83m, and Hg-206. Revision 3 provides the additional DRFs calculated using the same methods as used in Revision 2 of this document. The method for estimating new DRFs for the ELLWF disposal units is described in this report.

61 RADIATION PROTECTION AND DOSIMETRY↗

Soil Sampling Results for Closure of a Portion of Solid Waste Management Unit #16

This report presents the results of the sampling effort and documents all associated field activities including borehole clearing, soil sample collection, storage and transportation to the analytical laboratories, borehole backfilling and surface restoration, and storage of investigation-derived waste (IDW) for future profiling and disposal by SNL/CA waste management personnel.

54 ENVIRONMENTAL SCIENCES↗

PORFLOW Modeling of Vadose Zone Flow and Transport for E-Area Intermediate Level Vault

In support of the E-Area Performance Assessment, a two-dimensional model of water flow and radionuclide transport through the E-Area Intermediate Level Vault (ILV) and local vadose zone has been developed using the PORFLOW TM software. The purpose of the model is to calculate flux to the water table for radionuclides eluted from the ILV during its operational life, the period of institutional control, and times following site closure. Results of model calculations will be used by a three-dimensional PORFLOW model of transport through the aquifer to determine radionuclide concentrations at a hypothetical 100 meter well and at the site boundary where contaminated groundwater is accessible to members of the public following site closure.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Degradation and Upcycling of Poly(acrylic) Acid (PAA)

Poly(acrylic acid) (PAA) is a superabsorbent polymer (SAP) widely used in food, paint, textiles, and household products, such as absorbent hygiene products. Specifically, disposable diaper waste comprises a large majority of hygiene waste, in which 80% is landfilled and 20% is incinerated. This proposal describes new methods to valorize PAA to mitigate pollution and risk of large-scale release, dispersion, and accumulation of PAA into aquatic and terrestrial environments. The first strategy builds upon photoredox catalysis to oxidize PAA, which will allow for subsequent cleavage to PAA into valuable chemical feedstocks with intriguing functional groups that can readily undergo further transformations. Moreover, in conjunction with RAFT polymerization, photoredox catalysis would also lead to preparation of new graft block polymers to serve as pH-sensitive drug delivery vehicles. The second strategy invokes electrocatalysis, which can access different intermediates compared to photoredox catalysis. This method would lead to refunctionalization and repurpose of PAA into hydrogels and zwitterionic polymers that can find utilities in ion exchange, water treatment, soil conditioning, paper reinforcement, pigment retention, shampoo formulation, and drug delivery.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Assessment of Active Metal Removal from Pyroprocessing Salt by Electrodeposition

Active metals present in used nuclear fuel dissolve into the salt during pyroprocessing, but are not recovered during electrorefining or drawdown operations due to their chemical stability in the salt. The accumulation of 137 Cs and 90 Sr in process salt over time increases the heat load and ionizing radiation level of the salt such that it must be replaced frequently, resulting in a significant amount of salt waste. An effective means of removing active metals from the molten salt to enable recycle of the electrolyte (e.g., LiCl/KCl) would increase the efficiency of pyroprocessing and decrease the volume of salt waste requiring disposal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Recycled Paper as a Source of Renewable Jet Fuel in the United States

Converting biomass into jet fuel involves more than the core chemical process. The overall process includes the logistics of harvesting and transporting the biomass, handling and preparing the material for processing, and processing and disposal of waste. All of these activities contribute to cost. Controlling cost involves more than developing efficient process chemistry. Choice of feedstock also has a significant impact on process economics. We consider chemical conversion of paper from municipal solid waste as a feedstock for the production of jet fuel and diesel. Paper has a significantly higher cellulose content than raw lignocellulosic biomass such as corn stover, so it requires less pretreatment to convert it into hydrocarbons than lignocellulosic biomass. Our techno-economic analysis showed that the cost of converting paper waste into jet fuel is about $1.00/gal less than jet fuel produced from corn stover. Although the cost of recycling paper into jet fuel is less than producing it from corn stover, the process is not competitive with petroleum. We estimated a minimum selling price of $3.97/gal for paper-derived jet fuel. Our sensitivity studies indicated that the biggest economic obstacle is the cost of cellulose hydrolysis. Direct hydrogenation of paper to sugar alcohols combined with increased economy of scale could make recycling paper jet fuel competitive.

09 BIOMASS FUELS↗