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DOE OSTI2014

Formation of Interfacial Layer and Long-Term Cylability of Li-O-2 Batteries

Extended cycling of the Li-O2 battery under full discharge/charge conditions is achievable upon selection of appropriate electrode materials and cycling protocol. However, the decomposition of the side products also contribute to the observed good cycling behavior of high capacity Li-O2 batteries. Quantitative analyses of the discharge and charge products reveals a quick switch from the predominant formation of Li2O2 to the predominant formation of side products during the first a few cycles of the Li-O2 batteries. After the switch, cycling stabilizes with a repeatable formation of Li2O2/side products at ~1:2 ratio. CNTs/Ru composite electrodes exhibits lower charge voltage and deliver 50 full discharge-charge cycles without sharp capacity drop. Ru coated glass carbon electrode can lead to more than 500 cycles without change in its cycling profiles. The better understanding on Li-O2 reaction processes developed in this work may lead to the further improvement on the long term cycling behavior of high capacity Li-O2 batteries.

carbon nanotubes↗

DOE OSTI2020

Electrolytically Assisted Surface Decontamination (EASD{sup TM}) for POCO Operations - 20282

NNL in collaboration with C-Tech Innovation Ltd and Sellafield Ltd has been exploring innovative technologies to enable a significant reduction of radiological hazards within facilities during the Post Operational Clean Out (POCO) phase of a nuclear plant's life cycle. Reducing the hazard by effectively decontaminating plants in-situ during POCO delivers huge cost reductions for future decommissioning operations. These cost reduction benefits are realized by reducing the number and complexity of remote operations as well as lowering the long-term waste disposal costs. Whilst chemical decontamination can achieve the desired level of decontamination, applying aggressive chemical reagents is hazardous, potentially difficult to control and requires there to be complimentary effluent treatment and waste routes. This work has aimed to develop flexible and controllable decontamination processes which could be operated without the additional complexity and issues associated with chemical decontamination. The processes needed to be relatively fast and effective to minimize the time operators would spend in an active area. In addition, there was a driver to produce decontamination methodologies which generated a secondary waste compatible with current routes and which takes advantage of current waste capacity. The strategy therefore was to come up with a solution that works with, rather than against, the science and engineering behind process plants at Sellafield. Electrolytically Assisted Surface Decontamination (EASD{sup TM}) is an innovative electrochemical decontamination process (developed by NNL and C-Tech Innovation Ltd) that can remove activity from contaminated metal in very short time periods. Application of the patented electric waveform to the surface when treating contaminated metal with nitric acid has been shown to significantly enhance the decontamination performance. When compared to proposed baseline washout procedures at Sellafield, the only change to the process is the applied electrical waveform which is temporary and controllable. The current causes dissolution of the metal surface being decontaminated which leads to activity transferring from the plant item into the nitric acid effluent stream. This innovation has the potential to transform the POCO process and allow a nitric acid based washout approach to deliver POCO quickly and cost effectively within the existing infrastructure. Several devices have now been designed that incorporate this EASD{sup TM} technology and enable the decontamination process to be applied to a range items commonly identified as being contaminated during nuclear decommissioning programmes such as pipework, tanks and hotspots of walls/floors. Inactive and active laboratory-scale testing has been completed using both simulated and 'real-life' contaminated (low level waste) metallic items retrieved from different nuclear sites. Active trials demonstrated that contaminated items could be treated to free release levels within minutes. Engineering scale tests are currently being performed, with guidance from Sellafield's system engineers and plant managers, to provide the necessary re-assurance the designed devices could be successfully deployed in an on-plant scenario. The final stage of this development work is to carry out an active demonstration of the decontamination technology on Thorp at Sellafield. This paper aims to highlight progress made to date with the EASD{sup TM} technology and, more specifically, the development of an in-situ decontamination device for deployment within radioactive pipework. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2018

Basic properties of eutectic chloride salts NaCl-KCl-ZnCl 2 and NaCl-KCl-MgCl 2 as HTFs and thermal storage media measured using simultaneous DSC-TGA

Concentrated solar power (CSP) technologies tend to work at high temperatures for better energy efficiency, which need high temperature heat transfer fluids (HTF) and thermal storage. A good HTF should have low melting point and be thermally stable at high temperatures. A thermal storage medium needs a high heat capacity in order to store more energy in per unit of mass or volume. The objective of this work is to study the basic thermophysical properties of several eutectic molten salts for HTF and thermal storage media, which can work at upper limit temperatures of 850 °C. The eutectic salts are mixtures by NaCl-KCl-ZnCl 2 , and by NaCl-KCl-MgCl 2 , respectively. The heat capacity, melting point, and heat of fusion of the eutectic salts at different temperatures were measured using Differential Scanning Calorimetry (DSC) and Thermal Gravimetric Analysis (TGA) simultaneously. Details of the measurements and obtained experience of operating the equipment are provided in the work. For each of the eutectic salts multiple samples were tested to check repeatability and to minimize random errors. Finally, in theoretical analysis, mixing rules from literature was used to estimate the heat capacity of the new HTFs, which showed good agreement with experimental data.

14 SOLAR ENERGY↗

DOE OSTI2019

Implications of water constraints on electricity capacity expansion in the United States

The development of new electricity generation capacity is constrained by water resource availability. However, the sufficiency of available water resources is rarely incorporated into the planning of electricity capacity expansion in the United States. Previous studies on the implications of water constraints on US electricity generation are limited in terms of scale and robustness. Here, we extend previous studies by including physical water constraints within a state-level model of the US energy system embedded within a global integrated assessment model (GCAM-USA) that integrates both supply and demand effects under a consistent framework. We show that water constraints have two general effects across the United States: (1) to increase the cost of electricity generation, which results in slightly reduced electrification of end-use sectors, and (2) to incentivize early retirement of water-intensive technologies before the end of their designed lifetimes, while simultaneously boosting investment in less water-dependent technologies. Our results suggest that water availability constraints may cause substantial capital stock turnover and result in non-negligible economic costs for the western United States, whereas fewer impacts may be anticipated in the eastern United States. Our work emphasizes the need to integrate water availability constraints into electricity capacity planning and highlights the state-level challenges to facilitate regional strategic resource planning.

Liu, Lu↗

DOE OSTI2023

The Mechanism of Fluorine Doping for the Enhanced Lithium Storage Behavior in Cation-Disordered Cathode Oxide

Li-rich cation-disordered rock-salt (DRX) materials have emerged as promising candidates for high-capacity oxide cathodes. Their fluorinated variants have shown improved cycling stability with effectively suppressed oxygen loss. However, a comprehensive understanding of how fluorination impacts the multiscale structure and lithium transportation in DRX remains elusive in experiments. In this study, the neutron total scattering technique in conjunction with the advanced reverse Monte Carlo (RMC) fitting method is employed to characterize the intricate structure of Li 1.16 Ti 0.37 Ni 0.37 Nb 0.1 O 2 (LTNNO) and the fluorinated Li 1.2 Ti 0.35 Ni 0.35 Nb 0.1 O 1.8 F 0.2 (LTNNOF). Through rigorous statistical analysis, the multiscale structural evolution upon fluorination is quantified from atomic (≤5 Å) to long-range scale (≈100 Å). The local Li-rich environments around F induce a modest 2.4% increment in the number of fast Li 0TM (transition metal) channels. Crucially, at a broader scale, the proportion of 0TM channels participating in percolation increases significantly from 2.9% in LTNNO to 8.7% in LTNNOF. Fluorination improves the capacity release mainly through merging isolated fast Li channels into the percolation network. This work experimentally unravels the multiscale mechanism of fluorination-induced performance improvement in DRX materials and highlights the necessity of adopting an advanced RMC fitting method to obtain a full view of the complex structural features in developing high-capacity DRX cathodes.

25 ENERGY STORAGE↗

DOE OSTI2024

First-principles investigation of the thermophysical properties of NaCl, PuCl 3 , and NaCl-PuCl 3 Molten salts

Molten salts have a variety of applications that span the nuclear and solar industries, and which involve thermal storage and heat transfer. There is a present knowledge gap in the thermophysical properties of molten salts, which limits the readiness level of molten salt applications. This is especially pertinent for molten salt reactors where the fissile material is dissolved within the molten salt. Ab initio molecular dynamics is a common method employed to investigate the structural and thermophysical properties at elevated temperatures. NaCl-PuCl 3 is a candidate fuel salt in molten salt reactors. The scope of this study is to investigate the seven unique compositions and a range of temperatures of NaCl-PuCl 3 and calculate the density, heat capacity, compressibility, enthalpy of mixing, and coefficient of thermal expansion. Within this work, the van der Waals (vdW) interactions are primarily handled with the vdW-DF2 functional but spot-checked with both the dDsC and DFT-D3 methods. The calculated densities are in good agreement with the NaCl and the eutectic compositions, and no experimental values exist for PuCl 3 at these temperatures. The densities are fit to a first-order Redlich-Kister expansion as a function of both composition and temperature. The heat capacity in the literature is scattered but the calculated values agree well with one of the experimental results. Here, the heat capacity increases as a linear function with respect to concentration at a rate of about 7.5 J/mol-K per 10 mol% PuCl 3 .

36 MATERIALS SCIENCE↗

DOE OSTI2025

Benchmark of numerical modeling approaches on the systematic performance evaluation of wave energy converters

Different numerical modeling methods have been developed and applied to evaluate a variety of performance indicators of wave energy converters (WECs), including the power performance, structural loads, levelized cost of energy, etc. Based on the modeling fidelity, the commonly used numerical modeling approaches can be classified as linear modeling, weakly nonlinear modeling and fully nonlinear modeling approaches. Each method differs in accuracy and computational efficiency, making them suitable for different stages of WEC design. However, the selection of modeling approach could significantly impact evaluation outcomes. For instance, simplified linear models may underestimate structural loads or overestimate energy production in some operational conditions, potentially leading to less cost-effective designs. Given the widespread utilization of these models, it is essential to understand the uncertainties brought by them in performance evaluations. This work is dedicated to benchmarking different linear-potential-flow-based numerical models for evaluating the systematic performance of WECs. Three representative numerical modeling approaches are considered in this work, including linear frequency-domain modeling, statistically linearized spectral-domain modeling and Cummins equation-based nonlinear time-domain modeling. A generic point absorber WEC is considered as the research reference in this work, and different sea sites are taken into account. The numerical models are utilized to predict critical performance indicators, including power performance, the annual energy production, the capacity factor, the levelized cost of energy and the PTO fatigue loads. By comparing the results, this work identifies the uncertainties associated with different modeling approaches in evaluating WEC performance.

Fatigue↗

NASA NTRS2017

Preliminary Investigation of Impact of Technological Impairment on Trajectory-Based Operations

The Next Generation Air Transportation System (NextGen) incorporates collaborative air traffic management and Trajectory-Based Operations (TBO) in order to significantly increase the capacity, efficiency, and predictability of operations in the National Airspace System (NAS), without decreasing safety. This is enabled by airspace users and service providers sharing knowledge about operations that allows prediction of the complete 4D flight trajectory with as little uncertainty as possible. Additionally, new software and hardware technology is critical to reaching NextGen goals, especially with regard to TBO. What if the technologies that are critical for TBO were to be impaired or fail completely? Should there be a malfunction of a piece of the technology, it must be ensured that the whole system does not break down completely or suffer severe impairment. Instead, operations need to be maintained proportionally to the problem and safety needs to be ensured (graceful degradation). This paper proposes a systematic framework to investigate the vulnerability of TBO to technology disruption, and determine the impact of technological impairment on TBO. Two representative technologies are chosen for detailed investigation and the impact of their impairment on the degradation of TBO is illustrated using a weather-related scenario. XXXX There are several possible directions of future work. We believe it is desirable to develop methods to quantitatively assess the impact of technological disruption on TBO and to have the simulation tools to validate the impact. The availability of prognostics and health management methods could be leveraged to predict technological failure/disruption, thus predicting how TBO will be a ected, and possibly pro-actively mitigating the impact. It is important to develop large-scale scenarios where the e ect of technological impairment is prominent, and identify methods to quantitatively assess the extent of TBO degradation. An important goal of such an investigation is the development of failure-resistant resilient trajectory-based oper- ations. Resilience14, 15 is the property of a system to \bounce back" and resume at least a signi cant portion of its functionalities after degradation due to technological impairment(s). A systems resilience includes properties such as \bu ering capacity" (quantifying disruptions the system can absorb or adapt to without a fundamental breakdown in performance or in the systems structure), \ exibility" (ability to restructure itself in response to external changes or pressures), "margin" (how closely the system is currently operating rela- tive to one or another kind of performance boundary), \tolerance" (whether the system gracefully degrades as stress/pressure increase, or collapses quickly when pressure exceeds adaptive capacity), etc. Future work needs to focus on quantifying and improving the resilience of TBO, and identifying resilient design solutions for aviation.

TBO↗

DOE OSTI2022

Pilot Testing of a Highly Efficient Pre-combustion Sorbent-based Carbon Capture System

TDA developed and demonstrated a highly efficient pre-combustion carbon capture system. The overall objective of this work was to develop a new sorbent-based pre-combustion carbon capture technology for Integrated Gasification Combined Cycle (IGCC) power plants. In this project our goal was to demonstrate the techno-economic viability of the new technology by 1) demonstrating it in large-scale slipstream tests, and 2) carrying out a high fidelity engineering and cost analysis. TDA’s process used an advanced physical adsorbent that selectively removes CO 2 from coal-derived synthesis gas above the dew point of the gas at temperatures as high as 300°C. The sorbent consists of a mesoporous carbon whose surface was grafted with functional groups that remove CO 2 via a well-known acid-base interaction. As documented in bench-scale experiments and field tests with actual coal gas, the sorbent achieved a very high capacity for CO 2 at temperatures as high as 300°C. The sorbent bound CO 2 more strongly than common physical adsorbents, providing the chemical potential needed for the high temperature operation. However, because CO 2 does not form a true covalent bond with the surface sites (as is the case with chemical absorbents), the sorbent regeneration could be carried out with only a very small energy input. The heat input to regenerate our sorbent was only 4.9 kcal per mol of CO 2 , which is much lower than that for chemical absorbents (e.g., 29.9 kcal/mol CO 2 for sodium carbonate) and was similar to the requirements of physical solvents (e.g., 4 kcal/mol CO 2 for Selexol TM ). Because the sorbent operates above the dew point of the synthesis gas (unlike the Selexol TM process), a higher power cycle efficiency can be achieved. With previous DOE/NETL funding (Contract No. DE-FE-0000469), we demonstrated the techno-economic viability of the technology in bench-scale tests and slipstream demonstrations at the National Carbon Capture Center (NCCC), Wilsonville, Alabama and Wabash River IGCC plant in Terra Haute, Indiana. We demonstrated a stable working CO 2 capacity for over 11,650 cycles with simulated synthesis gas. We also evaluated its performance with actual synthesis gas in two test campaigns at the Wabash River IGCC Plant, Terre Haute, IN and the National Carbon Capture Center (NCCC), Wilsonville, AL. The slipstream tests clearly showed that the actual coal gas constituents and potential contaminants (e.g. trace metals, halides, tars) had no effect on the sorbent’s ability to remove CO 2 (the same sorbent beds were used in both field tests with no sign of deactivation for 2,000 cycles with over 26,750 SCF of gas treated). As expected, due to the high temperature CO 2 removal capability and low energy needed to regenerate the sorbent, the power cycle efficiency with our process was greater than 34% on a higher heating value (HHV) basis; in comparison, the same IGCC plant equipped with the Selexol TM solvent for carbon capture can only achieve 31.4% HHV efficiency. The capital cost for an IGCC system with TDA’s process is estimated as $2,417/kW e , which is 12% lower than that of the IGCC/ Selexol TM process. The levelized cost for electricity including the transport, storage and monitoring (TS&M) cost for CO 2 was calculated as $\$ $92.9/MWh (lowest reported to our knowledge), which is much better than the $105.2/MWh estimated for the IGCC/ Selexol TM process. In this project (DE-FE0013105), TDA Research, in collaboration with our partners Gas Technology Institute (GTI), Illinois Clean Coal Institute (ICCI), University of California, Irvine (UCI), University of Alberta (UOA), Siemens, NCCC and Sinopec advanced the technical maturity of the technology; scaling it up by a factor of 100. We optimized the reactor design using computational fluid dynamics (CFD); using adsorption modeling we improved the pressure swing adsorption (PSA) cycle sequence. We carried out two field test campaigns with a fully-equipped 0.1 MW e prototype unit (for a total of 844 hours) using actual synthesis gas to prove the viability of the new technology. A successful 30 day (707 hrs) evaluation was completed at NCCC under air blown gasification conditions. We demonstrated 97.3% carbon capture at 1,500 SLPM, 93% carbon capture at 1,800 SLPM, and 90% carbon capture at 2,100 SLPM in the NCCC tests. We also demonstrated the system for 137 hours at a Sinopec petrochemical plant under oxygen blown gasification, demonstrating 86% carbon capture at 2,660 SLPM. In collaboration with University of California, Irvine (UCI), we completed a techno-economic analysis (TEA) for TDA’s warm gas cleanup technology integrated to IGCC power plant. The net plant efficiencies (on a coal HHV basis) for the warm gas cleanup cases were estimated to be 34.0% for E-GasTM gasifier, 34.4% for GE gasifier, 33.4 for the Shell gasifier and 34.2 for the TRIG TM gasifier (Cases 2, 4, 6 and 8 in this study) with a catalytic combustor for CO 2 purification, which are significantly higher than those for the Cold Gas Case, or an increase of as much as 12% in the heat rate for Case 2, 6% for Case 4, 9% for Case 6, and 9% for Case 8. The 1st year cost of electricity with the transport, storage and monitoring (TS&M) costs for the CO 2 included was $\$ $129.2/MWh for the E-GasTM gasifier Warm Gas Cleanup Case, $\$ $131.9/MWh for the GE gasifier Warm Gas Cleanup Case, $\$ $146.8/MWh for the Shell Gasifier Warm Gas Cleanup Case, and $\$ $129.9/MWh for the TRIG TM gasifier Warm Gas Cleanup Case. For comparison, the costs for the baseline Cold Gas CO 2 removal with Selexol for the different gasifiers were: $\$ $146.6/MWh for the E-Gas TM gasifier, $\$ $142.2/MWh for the GE gasifier, $\$ $159.0/MWh for the Shell gasifier and $\$ $144.3/MWh for the TRIG TM gasifier. In summary, the costs for our system were 7 to 12% lower than the corresponding Cold Gas Cleanup cases. The results of this techno-economic analysis suggested that TDA’s high temperature PSA-based Warm Gas Clean-up Technology can make a substantial improvement in the IGCC plant thermal performance for achieving near zero CO 2 emissions for E-Gas TM , GE, Shell and TRIG TM gasifier based IGCC power plants. The capital expenses were estimated to be lower than that of Selexol’s™. Taken together, the higher net plant efficiency and lower capital and operating costs resulted in substantial reduction in the cost of carbon capture for the IGCC plant equipped with TDA’s high temperature PSA-based carbon capture system. Finally, in collaboration with Gas Technology Institute (GTI) we completed the environmental health and safety assessment for TDA’s warm gas carbon capture technology.

01 COAL, LIGNITE, AND PEAT↗

NASA NTRS1992

A procedure for sizing propulsion system filter capacity

A propulsion system filter has the function of protecting downstream components from propellant-borne particulate matter. A the same time, it must be designed with sufficient capacity to ensure that it will not clog during the life of the spacecraft. This capacity can be quantitatively calculated by means of the procedure described here. Previous work has presented limited data which suggest that filter clogging is a function of the number and size of ingested particles. Cleaning specifications for propusion system components are also normally given in terms of the number and size of particles removed by the flow of test fluid. It is proposed here that the filter capacity be given in terms of the number and size of particles, which in turn may be convected to an equivalent quantity of test dust.

Jan, Darrell L.↗

DOE OSTI2022

Viability of S3 Object Storage for the ASC Program at Sandia

Recent efforts at Sandia such as DataSEA are creating search engines that enable analysts to query the institution’s massive archive of simulation and experiment data. The benefit of this work is that analysts will be able to retrieve all historical information about a system component that the institution has amassed over the years and make better-informed decisions in current work. As DataSEA gains momentum, it faces multiple technical challenges relating to capacity storage. From a raw capacity perspective, data producers will rapidly overwhelm the system with massive amounts of data. From an accessibility perspective, analysts will expect to be able to retrieve any portion of the bulk data, from any system on the enterprise network. Sandia’s Institutional Computing is mitigating storage problems at the enterprise level by procuring new capacity storage systems that can be accessed from anywhere on the enterprise network. These systems use the simple storage service, or S3, API for data transfers. While S3 uses objects instead of files, users can access it from their desktops or Sandia’s high-performance computing (HPC) platforms. S3 is particularly well suited for bulk storage in DataSEA, as datasets can be decomposed into object that can be referenced and retrieved individually, as needed by an analyst. In this report we describe our experiences working with S3 storage and provide information about how developers can leverage Sandia’s current systems. We present performance results from two sets of experiments. First, we measure S3 throughput when exchanging data between four different HPC platforms and two different enterprise S3 storage systems on the Sandia Restricted Network (SRN). Second, we measure the performance of S3 when communicating with a custom-built Ceph storage system that was constructed from HPC components. Overall, while S3 storage is significantly slower than traditional HPC storage, it provides significant accessibility benefits that will be valuable for archiving and exploiting historical data. There are multiple opportunities that arise from this work, including enhancing DataSEA to leverage S3 for bulk storage and adding native S3 support to Sandia’s IOSS library.

96 KNOWLEDGE MANAGEMENT AND PRESERVATION↗

DOE OSTI2018

Electrical Conductivity and Electrochemical Characteristics of Na{sub 3}V{sub 2}(PO{sub 4}){sub 3}-Based NASICON-Type Materials

NASICON-type materials with the compositions Na{sub 3}V{sub 2–x}Al{sub x}(PO{sub 4}){sub 3}, Na{sub 3}V{sub 2-} {sub x}Fe{sub x}(PO{sub 4}){sub 3}, Na{sub 3+} {sub x}V{sub 2–x}Ni{sub x}(PO{sub 4}){sub 3}, and Na{sub 3}V{sub 2-} {sub x}Cr{sub x}(PO{sub 4}){sub 3} (x = 0, 0.03, 0.05, and 0.1) have been prepared and characterized by X-ray diffraction analysis, electron microscopy, and impedance spectroscopy. The results demonstrate that the highest electrical conductivity among the samples studied is offered by the material doped with 5% Fe: Na{sub 3}V{sub 1.9}Fe{sub 0.1}(PO{sub 4}){sub 3}. The activation energy for low-temperature conduction in the doped materials decreases from 84 ± 2 to 54 ± 1 kJ/mol and that for high-temperature conduction is ~33 kJ/mol. The discharge capacity of Na{sub 3}V{sub 1.9}Fe{sub 0.1}(PO{sub 4}){sub 3}/C under typical working conditions of cathodes of sodium ion batteries has been shown to exceed that of Na{sub 3}V{sub 2}(PO{sub 4}){sub 3}/C. The capacity of the more porous material prepared by the Pechini process (Na{sub 3}V{sub 1.9}Fe{sub 0.1}(PO{sub 4}){sub 3}/C-{II}) approaches the theoretical one at a low charge–discharge rate and retains its high level as the charge rate is raised (its discharge capacity was 117.6, 108.8, and 82.6 mAh/g at a discharge rate of 0.1C, 2C, and 8C, respectively).

25 ENERGY STORAGE↗

DOE OSTI2013

Improving the Estimates of Waste from the Recycling of Used Nuclear Fuel - 13410

Estimates are presented of wastes arising from the reprocessing of 50 GWD/tonne, 5 year and 50 year cooled used nuclear fuel (UNF) from Light Water Reactors (LWRs), using the 'NUEX' solvent extraction process. NUEX is a fourth generation aqueous based reprocessing system, comprising shearing and dissolution in nitric acid of the UNF, separation of uranium and mixed uranium-plutonium using solvent extraction in a development of the PUREX process using tri-n-butyl phosphate in a kerosene diluent, purification of the plutonium and uranium-plutonium products, and conversion of them to uranium trioxide and mixed uranium-plutonium dioxides respectively. These products are suitable for use as new LWR uranium oxide and mixed oxide fuel, respectively. Each unit process is described and the wastes that it produces are identified and quantified. Quantification of the process wastes was achieved by use of a detailed process model developed using the Aspen Custom Modeler suite of software and based on both first principles equilibrium and rate data, plus practical experience and data from the industrial scale Thermal Oxide Reprocessing Plant (THORP) at the Sellafield nuclear site in the United Kingdom. By feeding this model with the known concentrations of all species in the incoming UNF, the species and their concentrations in all product and waste streams were produced as the output. By using these data, along with a defined set of assumptions, including regulatory requirements, it was possible to calculate the waste forms, their radioactivities, volumes and quantities. Quantification of secondary wastes, such as plant maintenance, housekeeping and clean-up wastes, was achieved by reviewing actual operating experience from THORP during its hot operation from 1994 to the present time. This work was carried out under a contract from the United States Department of Energy (DOE) and, so as to enable DOE to make valid comparisons with other similar work, a number of assumptions were agreed. These include an assumed reprocessing capacity of 800 tonnes per year, the requirement to remove as waste forms the volatile fission products carbon-14, iodine-129, krypton-85, tritium and ruthenium-106, the restriction of discharge of any water from the facility unless it meets US Environmental Protection Agency drinking water standards, no intentional blending of wastes to lower their classification, and the requirement for the recovered uranium to be sufficiently free from fission products and neutron-absorbing species to allow it to be re-enriched and recycled as nuclear fuel. The results from this work showed that over 99.9% of the radioactivity in the UNF can be concentrated via reprocessing into a fission-product-containing vitrified product, bottles of compressed krypton storage and a cement grout containing the tritium, that together have a volume of only about one eighth the volume of the original UNF. The other waste forms have larger volumes than the original UNF but contain only the remaining 0.1% of the radioactivity. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

A Dendrite-Resistant Sodium/Porous-Carbon Anode for Solid-State Batteries – Strategies and Challenges for Low-Pressure Operation

Sodium solid-state batteries (Na-SSB) have gained interest recently due to the abundance of Na over Li, but they still tend to fail due to dendrites under practical current densities and cycling capacities. To overcome this, Na-SSBs are frequently tested with impractically high applied pressure. In this work, a porous carbon interfacial layer is utilized in conjunction with Na-ß”-Al2O3 solid electrolytes to enable Na-cycling at milder cell pressures. This sodium/porous carbon layer enables improved solid-state Na cycling in symmetric cells, up to a current density of 10 mA cm-2 at 25 °C. Cycling up to 1 mAh cm-2 is challenging with low pressure, but 1 mAh cm-2 capacity can be reliably cycled at 1 mA cm-2 at an elevated temperature of 60 °C in symmetric cells. Finally, the evolution of the interface and sodium/carbon anode is evaluated with cryogenic ion-milling and cross-sectional imaging revealing that, depending on testing temperature, pressure, current density, and capacity, void formation, Na-extraction from porous carbon, delamination of the porous carbon matrix, or a combination of these occurs at the interface between Na-metal and BASE. Despite this, excellent dendrite resistance is achieved, and a full-cell design utilizing a Na-transition metal oxide cathode is still able to achieve an areal capacity of ~ 2.7 mAh cm-2 at 0.125 mA cm-2. This work demonstrates an alternative pathway toward a Na-metal anode for Na-SSBs without the requirement of excessive stack pressure.

low-cost↗

NASA NTRS2016

Morton et al. Reply

Multiple mechanisms could lead to up-regulation of dry-season photosynthesis in Amazon forests, including canopy phenology and illumination geometry. We specifically tested two mechanisms for phenology-driven changes in Amazon forests during dry-season months, and the combined evidence from passive optical and lidar satellite data was incompatible with large net changes in canopy leaf area or leaf reflectance suggested by previous studies. We therefore hypothesized that seasonal changes in the fraction of sunlit and shaded canopies, one aspect of bidirectional reflectance effects in Moderate Resolution Imaging Spectroradiometer (MODIS) data, could alter light availability for dry-season photosynthesis and the photosynthetic capacity of Amazon forests without large net changes in canopy composition. Subsequent work supports the hypothesis that seasonal changes in illumination geometry and diffuse light regulate light saturation in Amazon forests. These studies clarify the physical mechanisms that govern light availability in Amazon forests from seasonal variability in direct and diffuse illumination. Previously, in the debate over light limitation of Amazon forest productivity, seasonal changes in the distribution of light within complex Amazon forest canopies were confounded with dry-season increases in total incoming photosynthetically active radiation. In the accompanying Comment, Saleska et al. do not fully account for this confounding effect of forest structure on photosynthetic capacity.

Morton, Douglas C.↗

DOE OSTI2017

Understanding the interacted mechanism between carbonation and chloride aerosol attack in ordinary Portland cement concrete

An experimental study is carried out with the aim to understand the interacted mechanism between carbonation and chloride aerosol attack in ordinary Portland cement (OPC) concrete. Effects of carbonation on the chloride profile, the chloride binding capacity and the chloride diffusion coefficient are evaluated. Besides, effect of chloride aerosol attack on the carbonation rate is investigated. Concrete specimens with three water-to-cement ratios (0.38, 0.47 and 0.53) are fabricated in this work. Tested results demonstrate that carbonation remarkably affects the chloride profile, reduces the chloride binding capacity, and also accelerates the rate of chloride ion diffusion of concrete. Besides, the presence of chloride aerosol can lead to lower the carbonation depth and increase the pH value of carbonated concrete. Microscopic properties such as morphology, porosity, and pore size distribution for the contaminated concretes are explored by scanning electron microscope and mercury intrusion porosimetry, which provide strong evidence to these research findings.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Lattice and Local Electronic Structure Modulation Enables Ultra-Long-Life Li-Rich Cathode Materials

Effectively alleviating severe performance deterioration including rapid capacity decay and continuous voltage fading of Li-rich layered oxide (LLO) cathodes by suppressing the irreversible oxygen release and transition metal (TM) migration is a critical challenge during prolonged cycling. Herein, we report a Sb-doped LLO (SLLO) cathode with shortened TM oct –TM oct distance and modulated local electronic structure, which can significantly enhance the oxygen vacancy formation energy and TM migration energy barriers. Therefore, the SLLO cathode showcases an impressive energy density of 1052 Wh kg –1 at 0.2 C and an outstanding rate capability of 214 mAh g –1 at 5 C with a remarkable capacity retention of 79.2% even after 1000 cycles. It should be pointed out that it exhibits greatly enhanced voltage stability with an outstanding voltage retention of 86.2% after cycling 1600 times at 10 C. In conclusion, this work provides a prototype for significantly enhancing the reversibility in electrochemical reactions of high-capacity layered cathode materials.

25 ENERGY STORAGE↗

DOE OSTI2016

High capacity of lithium-sulfur batteries at low electrolyte/sulfur ratio enabled by an organosulfide containing electrolyte

We present that lithium-sulfur (Li-S) battery is a promising energy storage technology to replace lithium ion batteries for higher energy density and lower cost. Dissolution of lithium polysulfide intermediates in conventional Li-S electrolytes is known as one of the key technical barriers to the development of Li-S, because it promotes redistribution and irreversible deposition of Li 2 S, and also forces large amounts of electrolyte to be used, shortening cycling life and driving down cell energy density. Recently, dimethyl disulfide as a functional co-solvent has been demonstrated to show an alternate electrochemical reaction pathway for sulfur cathodes by the formation of dimethyl polysulfides and lithium organosulfides as intermediates and reduction products. In this work, comprehensive studies show that this new pathway not only provides high capacity but also enables excellent capacity retention through a built-in automatic discharge shutoff mechanism by tuning carbon/sulfur ratio in sulfur cathodes to reduce unfavorable Li 2 S formation. Furthermore, this new electrolyte system is also found to enable high capacity of high-sulfur-loading cathodes with low electrolyte/sulfur (E/S) ratios, such as a stable specific capacity of around 1000 mAh g -1 using a low electrolyte amount (i.e, E/S ratio of 5 mL g -1 ) and highsulfur-loading (4 mg cm -2 ) cathodes. This electrolyte system almost doubles the capacity obtained with conventional electrolytes under the same harsh conditions. In conclusion, these results highlight the practical potential of this electrolyte system to enable high-energy-density Li-S batteries.

25 ENERGY STORAGE↗