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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Cryogenic Carbon Capture™ (CCC) Status Report

The Cryogenic Carbon Capture™ (CCC) process separates CO2 from light gases in essentially any continuous process. CCC cools the gases to the frost or desublimation point of CO2 (-100 to -135 °C), separates and pressurizes the solids, and warms all streams to produce a CO2-depleted stream at ambient pressure and a pure (99+%) pressurized liquid CO2 stream typically to about 150 bar, both at ambient temperature. The process also recovers all gas moisture and most gas impurities less volatile than CO2 (NOx, SOx, Hg, PM, UHC, CCC, etc.) in separable streams. CCC nearly eliminates refrigeration energy for sensible temperature changes through heat integration. CCC does require energy to change the CO2 phase from a mixed vapor to a pressurized fluid, which represents the minimum energy required of any process for this separation. CCC uses additional energy for turbomachinery inefficiencies, heat losses, moisture removal and overall process pressure drop. Aside from these real-world energy demands, CCC operates near the minimum energy required to perform this gas separation by minimizing stream recycling. CCC compresses CO2 as a liquid, which is one of several reasons it costs about about half as much and consumes about half as much energy as an amine process when using flue gases with about 15% CO2. The process also has several major additional advantages, including (a) it is a bolt-on retrofit technology that does not need steam or any modification of existing equipment, (b) it recovers water and nearly all pollutants in addition to CO2 from the flue gas, (c) it enables highly efficient and cost effective energy storage at grid scale and on time scales of minutes, (d) it enables NG storage if the energy storage option is used, and (d) it has a small footprint and is minimally disruptive to existing plants, requiring only electrical power and a gas source to operate. Sustainable Energy Solutions (SES) has scaled this technology through several levels, the largest of which captures nominally 1 tonne of CO2/day and is called the skid system. Skid system field tests include utility-scale power plants, cement plants, heating plants, and other utility or industrial sites that burn natural gas, biomass, coal, shredded tires, municipal waste, and combinations of these fuels. These field tests produced 95-99% CO2 capture with CO2 purities of 99+% and initial CO2 contents that range from 4 to 28%. SES currently seeks to scale the system to merchant scale (10-80 tonnes of CO2 per day). In the process of doing so, SES has demonstrated the potential for CCC to contribute to energy storage and direct air capture in innovative and cost-effective ways. This presentation discusses the overall process and highlights results from field and in-house tests. These include (a) measured CO2 capture rates and operating conditions from in-house and field tests, and (b) predicted utility-scale costs and energy demands. This discussion also includes the application of the CCC technology to energy storage and direct air capture.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2026

Nepheline constraint for hanford HLW glass

The present work was intended to expand the available HLW glass property-composition data relating to nepheline formation on CCC heat treatment and to develop improved models to predict nepheline formation that would allow processing of high waste loading high-Al HLW glass formulations at the WTP.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2026

Space Cooling: Recovery, Reuse, Recycling and Supply Chain Impacts

The global cooling sector has undergone tremendous growth in recent years, and cooling demand is projected to double or triple by 2050. Surging air conditioning demand will continue to be driven by increased populations, incomes and occurrences of extreme heat and humidity events. Cooling equipment growth has important pollution and material implications as they are made up of critical metals and precious raw materials - including ferrous metals, copper, aluminum and printed circuit boards composed of copper, silver, gold and palladium - that generate significant electronic waste at end-of-life. Air conditioning equipment also contains fluorinated gas (F-gas) refrigerants, which are potent gases that are thousands of times more heat-trapping than carbon dioxide (CO2). While recovery, reuse, and recycling strategies have been assessed for cold chain and refrigeration, there is currently limited analysis on how these strategies could be adopted for the global space cooling industry and potential supply chain implications. This paper aims to address this research gap by qualitatively evaluating product and material recovery, reuse and recycling frameworks from both demand and supply-side perspectives and with the support of cooling-specific case studies. It also focuses on quantitatively assessing potential energy, emissions and resource benefits of such strategies for space cooling equipment. This paper first analyzes how existing recovery, reuse and recycling frameworks can be applied to space cooling, with emphasis on the demand-side enablers (e.g., innovative business models, supporting policies and regulations) and changes in supply-side production network throughout the supply chain (e.g., design, production and distribution, end-of-life recovery) needed to overcome existing barriers. It will present case studies of innovative business models for space cooling technologies, including reuse and recycling, and how effective refrigerant reclamation and recovery programs have been operationalized. Lastly, the paper will highlight global modeling results of energy, emissions and material recovery from scenario analysis of selected strategies for air conditioners. The findings of this paper are intended to inform the development of product and material recovery, reuse and recycling strategies for a rapidly growing stock of space conditioning equipment by addressing existing organizational, economic and regulatory barriers and potential supply-chain bottlenecks.

Khanna, Nina↗
DOE OSTI2020

Transparent window film with embedded nano-shades for thermoregulation

Every year, more than 20% of the energy consumption in the United States and more than 10% of the global consumption is used towards HVAC (Heating, Ventilating, Air-Conditioning) systems in buildings. Although continued efforts in advancing renewable energy, efficient appliances, and smart building systems are desired, the most critical factors that cause extensive indoor energy consumption are thermal leakage and thermal waste generation. We demonstrate a smart window film that allows natural lighting with a clear view while blocking oblique incident sunlight to make the building interior cooler without using electricity or generating heat. Building upon the concept of, often overlooked, traditional window shades and privacy window films, we emphasize and elevate the application and impact of using magnetically arranged nanoscale material for energy conservation purpose in buildings. By embedding vertically aligned Ni flakes (VANF) in a polymer matrix film, nanoscale mirror array serve as shades to block the high-angled incident sunlight, blocking approximately 73% of total solar irradiance and bringing down the indoor temperature by 1.92 °C during the daytime in a model house while providing nearly 90% transparency. Global application was simulated by applying the respective solar angle and intensity at selected latitudes, indicating their potential. This passively energy-conserving smart film is a low cost, maintenance free, and simple product for users and easy-to-manufacture product for the industry.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Combustion Synthesis of Transuranic-doped Ceramics for Nuclear Waste Immobilization

Utilizing the devised SCS technique, crystalline transuranic-doped zirconate pyrochlores were formed for the first time without the need for a subsequent heating step. Typically, materials rapidly synthesized in a single-step self-sustaining exothermic reaction require further heating to induce crystallization and purify the product. The need for this secondary processing step can be attributed to factors such as an improper oxidizer to fuel ratio and the utilization of strong complexing compounds as fuels (i.e., reducing agents), all of which hinder complete combustion. The efficacy of the developed process was demonstrated by fabricating crystalline plutonium-doped Gd2Zr2O7 from solutions containing metal nitrates and urea in a properly tuned ratio

Burton-Allen, Janiya D.↗
DOE OSTI2020

Laboratory-Scale Melter Systems for Simulated and Real AP-107 Tank Waste - 20483

The Hanford Waste Treatment and Immobilization Plant (WTP) will process and stabilize waste that is stored in underground tanks on the Hanford Site. At the WTP, the tank waste will be combined with glass-forming and modifying additives to form an aqueous and solid mixture called melter feed, which will then be vitrified in joule-heated melters. A small-scale melter system, the continuous laboratory-scale melter (CLSM), is designed to operate with a continuous feeding process while periodically pouring glass product and collecting off-gas. Two CLSMs were constructed: one in a non-radioactive environment for processing waste simulants and another in a fume hood capable of handling radioactive material for processing actual Hanford tank waste. The waste sample received for vitrification in the CLSM was from Hanford tank 241-AP-107. Approximately 12 liters of melter-feed slurry was vitrified into 7 kilograms of glass product over the course of 10 hours of charging to the CLSM. The partitioning of technetium-99 in the product streams was used to calculate the technetium-99 recovery and help determine when the vitrification process had reached a steady state. The average single-pass retention of technetium-99 in the glass product was then calculated for the processing of AP-107 waste in the CLSM system. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Modelling uranium dioxide corrosion under repository conditions: A pore-scale study of the chemical and thermal processes

This paper investigates the corrosion behaviors of spent uranium dioxide (UO 2 ) fuel when placed in geological repositories. We performed pore-scale reactive transport simulations of the UO 2 corrosion process in a defective fuel rod with different orientations of breach or fracture on its clad. It is found that the corrosion rate has strong dependency on the breach orientation. The highest corrosion rate of UO 2 is calculated when the angle between the groundwater flow direction and the clad fracture reaches 180°. UO 2 corrosion simulations with different flow rates are compared. The results show the higher flow rate accelerates the corrosion of UO 2 fuel. The effect of pH on the corrosion process is also determined. It is indicated that higher pH can limit the corrosion of UO 2 by reducing the reaction rate. The dependence of reaction rate and time on reactive surface area is explored. Spent fuel with lower surface area demonstrates longer lifetime under corrosion conditions. A numerical model coupling thermal conduction and chemical reactions is developed to assess the impact of temperature on the process of UO 2 corrosion. The results show that higher temperature leads to larger corrosion rates for UO 2 . Here, the predicted reaction rates are higher in comparison with the isothermal results. Hence, our results can help improve the fundamental understanding of UO 2 corrosion in geological repositories for long-term storage of spent nuclear fuels and provide guidance for the safe operations and selection of appropriate repositories.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Recent progress in the design of the K-DEMO divertor

The preliminary conceptual design of the Korean fusion demonstration reactor (K-DEMO) with a major radius of 6.8 m and the fusion power of 2200 MW has been studied since 2012. The overall configuration of the K-DEMO divetor system based on the ITER-like water-cooled tungsten technology is a double-null type symmetric divertor subdivided into 32 toroidal modules for the vertical maintenance. A detached divertor scenario with impurity seeding was considered as the primary approach for the power exhaust to reduce the peak heat flux lower than the engineering limit of 10 MW/m 2 . The power exhaust performance at the scrap off layer was estimated by using UEDGE-2D code, a two-dimensional fluid transport code for collisional edge plasma and neutral species like N, Ne, and Ar. Particle and heat flux on inboard and outboard divertor targets were calculated for the detached cased depending on parameters such as the impurity seeding rate, pumping rate, and the pedestal density. On the other hand, a magnetic solution like X-divertor, snowflake divertor, and super X-divertor to expand the plasma wet area was considered for K-DEMO since the detached divertor increasing a radiation fraction by impurity seeding might be able to be unstable. However, the extremely high current of poloidal coils was required more than the engineering limit, 20 MA, to form magnetic field lines for the alternative divertors. Based on the physical calculation of the edge plasma, engineering analyses were carried out to find out the thermal and structural reliability. The thermo-hydraulic analysis confirmed thermal stability, whether all comprising materials are operating within their allowable temperature windows when the case of the peak heat flux is set to 10 MW/m 2 on the outboard divertor target. The response surface optimization method derived two optimal design candidates employing two kinds of heat sink materials, respectively: the reduced activation ferritic martensitic (RAFM) steel and CuCrZr alloy. Additionally, the drawbacks and merits of the two materials were definite. The optimal design with applying RAFM steel was vulnerable to withstand thermal and mechanical loads since low thermal conductivity caused too thin thickness of the heat sink. On the other hand, the CuCrZr alloy has critical drawbacks in terms of activation and radioactive waste despite its high thermal conductivity. Meanwhile, preliminary electromagnetic (EM) analysis was carried out to estimate the EM loads caused by the abnormal behaviors of plasma since EM loads are one of the most critical external loads for designing a DEMO divertor.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Experimental, Economic, and Environmental Assessment of Feedstock Gasification for High-Octane Fuel Production

Five economically advantaged biomass feedstocks identified in the US Department of Energy's 2016 Billion Ton Study were gasified and the syngas reformed at the bench scale to study the feedstock price-performance relationship. The distribution of reformed syngas compositions, heating values, and yields were similar across the different feedstocks and blends thereof, which ranged from inexpensive residual wastes to more expensive and higher quality biomass, revealing that feedstock performance was mostly insensitive to its price. Custom blended feedstocks produced syngas with characteristics resembling linear combinations of syngas from single-component feedstocks, supporting the ability to customize and predict blended properties based on single-feedstock data. A techno-economic analysis of specific feedstock costs for producing high-octane gasoline showed that miscanthus and forest residues were the most cost-effective. A field-to-wheels life-cycle assessment of greenhouse gas emissions showed that forest residues was the most environmentally benign feedstock of those studied.

09 BIOMASS FUELS↗
DOE OSTI2024

Extraction of Value-Added Products from Food Processing Waste Using Dimethyl Ether

Poster for 2024 Intern Poster Session. Food production waste can be valorized to create a circular economy. Traditional extraction methods require pretreatment of the sample through heating or cell disruption, but this contributes to a majority of the process's energy usage for wet biomass. Using dimethyl ether extraction can combine the dewatering and extraction processes into one to skip the pretreatment step while still maintaining similar extraction rates.

09 BIOMASS FUELS↗
DOE OSTI2024

Extraction of Value-Added Products From Food Processing Waste Using Liquid Dimethyl Ether

Technical presentation for 2024 Intern Poster Session. Food production waste can be valorized to create a circular economy. Traditional extraction methods require pretreatment of the sample through heating or cell disruption, but this contributes to a majority of the process's energy usage for wet biomass. Using dimethyl ether extraction can combine the dewatering and extraction processes into one to skip the pretreatment step while still maintaining similar extraction rates.

09 BIOMASS FUELS↗
DOE OSTI2023

Advanced biorefinery feedstock from non-recyclable municipal solid waste by mechanical preprocessing

Because of accelerated urbanization and the development of a global economy, a large quantity of municipal solid waste (MSW) has been collected and disposed of by the municipalities. Due to this drastic increase in the disposal of MSW, the need for its management is a must to preserve the environment. Currently, approximately 50% of the total MSW generated in the United States has been utilized through various recycling, combustion, and composting technologies, which means the remaining 50% is sent to landfill; this is often known as non-recyclable MSW (nMSW). As this nMSW is physically and chemically heterogenous and contains very high amounts of inorganic material, processing is required prior to using it as a biorefinery feedstock. Thus, this study focused on how mechanical preprocessing advanced the physical and chemical properties of nMSW. The physical and chemical properties were investigated in terms of particle size distribution, bulk density, ultimate and proximate analysis, and the higher heating value (HHV). The combustion properties were examined in terms of ignition temperature, peak heat release rate, and combustion efficiency. Results showed that the variability of physical and chemical properties of nMSW can be reduced by mechanical preprocessing. For example, the variability of the bulk density of the as-received nMSW was approximately 17.3% while it reduced to 5.8% when the sample size was reduced to 2 mm. Similarly, the variability of ash and HHV reduced from 49.2% to 11.0% and 13.4%–4.2%, respectively. Combustion thermograms showed that the size reduction positively improved the combustion properties. For example, 2 mm of spec sample started to ignite approximately 4 times earlier and took 6.5 folds less time to reach the peak heating rate compared to as-received nMSW. Overall, the mechanical preprocessing reduced the variability of physical and chemical properties in addition to the improvement of combustion behavior of the nMSW which is one step forward toward the biorefinery feedstock.

09 BIOMASS FUELS↗
DOE OSTI2024

Chemical recycling of mixed textile waste

Globally, less than 0.5% of postconsumer textile waste is recycled, with the majority incinerated or ending up in landfills. Most postconsumer textiles are mixed fibers, complicating mechanical recycling due to material blends and contaminants. Here, we demonstrate the chemical conversion of postconsumer mixed textile waste using microwave-assisted glycolysis over a ZnO catalyst followed by solvent dissolution. This approach electrifies the process heat while allowing rapid depolymerization of polyester and spandex to their monomers in 15 minutes. A simple solvent dissolution enables the separation of cotton and nylon. We assess the quality of all components through extensive material characterization, discuss their potential for sustainable recycling, and provide a techno-economic analysis of the economic feasibility of the process.

Science & Technology - Other Topics↗
DOE OSTI2020

TCCR Operational Summary and Optimization for Tank 9 Processing - 20314

Savannah River Remediation (SRR) manages and operates the liquid waste facilities at Savannah River Site (SRS) for the Department of Energy (DOE). Stored liquid waste is a complex mixture of insoluble solids (sludge) and soluble salts in an alkaline solution. SRR has deployed the Tank Closure Cesium Removal (TCCR) system, a tank-side ion exchange process, to remove radioactive cesium from salt waste and enable onsite disposal of the resulting decontaminated salt solution as low-level waste at the Saltstone facilities. The TCCR system consists of two prefilters, four ion exchange (IX) columns, one resin trap, and a ventilation system. The IX process uses a form of inorganic crystalline silicotitanate (CST), which has a high affinity for cesium and other alkali metals, strontium, and actinides. This process is currently deployed utilizing salt feed from Tank 10, with future plans to dissolve solid salt in Tank 9 and transfer the salt solution to Tank 10 for processing through TCCR. The feed for TCCR must be created from salt-cake in Tank 10 through a dissolution process. Once enough salt has been dissolved, a qualification process is entered. This process characterizes the feed and ensures the cesium loading on the columns will not cause boiling of waste within the columns during or after processing. Once the batch has been qualified, salt waste is fed to the TCCR system through a transfer pump in the center of the tank. The waste is filtered through a set of two shielded, dead-end prefilters that prevent solids buildup in the columns. The filtered salt solution then travels to the shielded IX columns, which can be operated individually or in series, where the cesium is sorbed on the CST media. The decontaminated salt solution (DSS) then travels through a resin trap and out of the module to Tank 11. TCCR has successfully processed approximately 795,000 L of Tank 10H radioactive salt waste over two batches to date. There has not yet been a system induced shutdown. The prefilters performed as expected with only minor degradation in recovery of differential pressure after a backflush sequence. The time between backflushes decreased as each batch reached the end of processing. The hydraulics in the IXCs mostly performed as expected at all flow rates, except for one IXC that will be further investigated during Batch 3 processing. The TCCR system has shown some opportunities for more efficient processing during the length of the demonstration so far. For future processing of material from Tank 9H through Tank 10H and the TCCR unit, TCCR 1A will implement changes to the prefilters and the IXCs. The prefilters will have an increased surface area and a new filter media in an effort to increase time between filter swaps and improve backwashing cleaning capability. The IXCs will have a reduced diameter to allow for increased heat transfer out of the column and increased loading of Cs-137. Additionally, a new form of CST with an increased kinetic performance is being investigated for use during TCCR 1A operation. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

EBS Task Force: Task 9/FEBEX Modeling Final Report: Thermo-Hydrological Modeling with PFLOTRAN

This report outlines Sandia National Laboratories modeling studies applied to Stage 1 and Stage 2 of the Full-scale Engineered Barriers Experiment in Crystalline Host Rock (FEBEX) in situ test for the SKB EBS Task Force Task 9. The FEBEX test was a full-scale test conducted over ~18 years at the Grimsel, Switzerland Underground Research Laboratory (URL) managed by NAGRA. It involved emplacing simulated waste packages, in the form of welded cylindrical heaters, inside a tunnel in crystalline granitic rock and surrounded by a bentonite barrier and cement plug. Sensors emplaced within the bentonite monitored the wetting-up, heating, and drying out of the bentonite barrier, and the large resulting data set provides an excellent opportunity for validation of multiphysics Thermal-Hydrological (TH), Thermal-Hydrologic-Chemical (THC), and Thermal-Hydrological-Mechanical (THM) modeling approaches for underground nuclear waste storage and the performance of engineered bentonite barriers. The present status of the EBS Task Force is finalizing Task 9, which follows years of modeling studies of the FEBEX test, by many notable modeling teams (Gens et al., 2009; Sanchez et al. 2010; 2012; Samper et al., 2018). These modeling studies generally use two-dimensional axisymmetric meshes, ignoring threedimensional effects, gravity and asymmetric wetting and dry out of the bentonite engineered barrier. This study investigates these effects with use of the PFLOTRAN THC code with massively parallel computational methods in modeling FEBEX Stage 1 and Stage 2 results. The PFLOTRAN numerical code is an open source, state-of-the-art, massively parallel subsurface flow and reactive transport code operating in a high-performance computing environment (Hammond et al., 2014). Section 2 describes the applied partial differential equations describing mass, momentum and energy balance used in this study, considerations derived by assuming phase equilibrium between gas and liquid phases, constitutive equations for granite, cement plug, and bentonite domains, and specific approaches for use inthe PFLOTRAN code. Section 3 describes the geometry, meshing, and model set-up. Section 4 describes modeling results, Section 5 compares modeling results to field testing data, and Section 6 gives conclusions. The Appendix provides detailed information required by the EBSTask Force for final reporting.

42 ENGINEERING↗
DOE OSTI2025

Vitrification Testing of HLW with High Phosphate

Projections of the number of high level waste (HLW) canisters to be produced in the Hanford Tank Waste Treatment and Immobilization Plant (WTP) (e.g., [1]) are based upon the inventory of the tank wastes, the anticipated performance of the sludge treatment processes, and current understanding of the capability of the borosilicate glass waste form. The WTP HLW melter design, unlike earlier Department of Energy (DOE) melter designs, incorporates a glass bubbler system. The bubblers create active glass pool mixing and thereby improve heat and mass transfer and glass melting rate. The WTP HLW melters each have a glass surface area of 3.75 m 2 and depth of ~1.1 m. The two melters in the HLW facility together are designed to produce up to 7.5 MT of glass per day at 100% availability. Further increases in HLW waste processing rates can potentially be achieved by optimization of the feed and glass formulations, increasing the melter operating temperature above 1150⁰C, and by increasing the waste loading in the glass product. Increasing the waste loading also has the added benefit of decreasing the number of canisters for storage.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Laboratory-Scale Coal-Derived Graphene Process (Final Report)

The Energy & Environmental Research Center (EERC) conducted a laboratory-scale coal-derived graphene (CDG) project focused on developing a technological process for making graphene from four U.S. domestic coal or coal wastes, including lignite from North Dakota, subbituminous coal from Wyoming, bituminous coal from Utah, and anthracite from Pennsylvania. The project was divided into two performance or budget periods (BPs), with BP1 comprising the up-front laboratory experiments to make graphene materials from coal beginning on May 1, 2020, to April 30, 2022. BP2 was conducted from May 1, 2022, to April 30, 2023, and was focused on analyzing the CDG process economic feasibility and the technical gaps for technological scale-up and commercialization. During this project, a few different coal-derived high-value products have been demonstrated, including graphite, graphene oxide (GO), reduced graphene oxide (rGO), and graphene quantum dots (GQDs). A new graphite microstructure was discovered and named “croissant graphite” because of the exterior morphological and textural resemblance to croissant food items sold in commercial groceries stores. The new graphite structure and the associated preparation from coal or coal waste feedstocks has been the subject of a U.S. patent application. The systematic experimental processes involving coal cleaning, upgrading, and conversion to high-value carbon products culminated into a developed upgraded coal-to-products (UCP) technology that is being pursued for potential fast-track commercialization, if funding is available. It is envisioned that commercialization of the UCP technology would increase consumption of U.S. domestic coals or coal wastes to make environmentally sustainable high-value products for the electronics industry, high-energy-storage applications, and clean energy technologies such as electric vehicle (EV) lithium-ion batteries (LIBs), for which graphite has become a critical mineral commodity. Croissant graphite microstructures, when observed by field emission scanning electron microscopy (FESEM), display wavy surface morphology and often grow from a base that is made of graphitized particles with honeycomb-like layers, which are believed to be graphene layers. While more studies are needed to fully ascertain the mechanisms of the croissant graphite microstructure formation, it is postulated that their growth may begin from curling of the graphene sheets into ribbon-like structures, and continuous growth and densification of the ribbon-like structures forms croissant microstructures. Additional studies are ongoing to evaluate the electrochemical performance of croissant graphite for LIB applications and to determine the experimental conditions necessary to tune on/off croissant formation so that it can be either optimized or suppressed depending on performance evaluation results. In addition to the discovery of croissant graphite, the graphitization process from the four coal ranks in general was successful. X-ray diffraction (XRD) analysis showed that the degree of graphitization (DoG) ranged from 12% to 80% in an early sample set, and further optimization on lignite coal produces a DoG of about 92%, which was spectacular to see as lignite is the lowest-rank coal. Thus, it is expected that the graphitization performance for higher-rank coals will be similar or better when optimized as well. The coal-derived graphite was used to make GO and rGO. Analytical characterization, e.g., by methods such as Raman spectroscopy, XRD, Fourier transform infrared (FTIR) spectroscopy and FESEM, showed that the sequence of converting the coal to graphite, exfoliating it to GO, and then chemically reducing the GO to rGO was successful. Although coal naturally contains aromatic compounds and some relatively small-sized condensed aromatic units, it does not contain graphene sheets. In the UCP process, the aromatic domains in the coals, particularly low-rank coals, are concentrated and condensed further into graphene sheets, which are ordered into a 3D stack during graphitization. The synthesized graphite is then unpacked by methods such as exfoliation to various graphene products. GQDs were synthesized from all four coal types, and their optical properties were demonstrated to be tunable by the coal precursor preprocessing treatments. In all four coal types, enhanced optical properties were observed for the produced GDQs with incremental improvements made to the coal precursors. GQDs produced from raw coal samples displayed lower ultraviolet–visible (UV–Vis) spectroscopy absorbance intensity compared to those obtained from cleaned and upgraded coal residues. The photoluminescence (PL) intensities also varied with pretreatment conditions and with the concentration of GQDs in aqueous solutions. GQDs obtained from anthracite show longer emission wavelengths and can be excited by visible light as opposed to GQDs derived from the other coal ranks. UV fluorescence 3D maps and spectra revealed that the emission wavelength at which the GQDs solutions display the highest intensity was slightly redshifted based on the coal precursor pretreatments. In low-rank coal (lignite and subbituminous) samples, two clusters were observed in the maps for GQDs, which may suggest that there are potentially two types of fluorophores in solution or two main size populations. The ability to tune the properties of GQDs based on processing methods can be exploited to make GQDs for various optical display or optoelectronics applications. The results also highlight the importance of removing coal-borne impurities to improve the quality of the coal precursor for preparation of graphene products. Coal and/or coal wastes preprocessing methods were developed and applied to clean and upgrade the coal precursors prior to graphitization and subsequent conversion to graphene products. The preprocessing methods involve high specific-gravity separations, mineral acid cleaning (no hydrofluoric acid), and subsequent upgrading by reducing the coal-borne heteroatom (nitrogen, sulfur, and oxygen) content using proprietary chemical agents. Analytical characterization revealed that the preprocessing steps were successful, with ash reductions that range from 38% to 80% and residual ash content that was below the 5 wt% initial target. Based on proximate and ultimate analysis, the heteroatom reduction reactions produced upgraded coal residues with the oxygen content reduced by 8% to 24%, with additional reductions in the nitrogen and sulfur contents. An initial assessment of the waste streams from the UCP process shows very small to negligible environmental impact due to CO 2 , NO x , and SO x because most process steps are performed under inert atmosphere with argon. Consequently, reactive oxygen environments that tend to create these species are avoided. The inorganic and potentially hazardous species are released into aqueous waste streams that are easy to handle for proper disposal. The liquid waste streams were found to contain low-level concentrations of rare-earth elements (REEs), which could be concentrated and recovered as value-added by-products. Additionally, the volatile and gaseous fractions from carbonization and heat treatment contain useful organic compounds that can also be recovered as potential valuable by-products. Thus, the UCP technology is considered an environmentally sustainable and promising emerging technology for making high-value products from coal and coal wastes, with potential additional value-added by-products. Analysis of potential markets for the coal-derived carbon products shows a strong demand in both niche market sectors and across a wide variety of other industrial sectors. Graphite is currently considered a critical mineral commodity that has a large and growing demand in the LIB industry for EV applications. Based on data from Fortune Business Insights (2022) and Marketwatch (2023) reports, the average global graphite market is projected to reach about 33 billion by 2028, growing at a compound annual growth rate (CAGR) of about 7%, with much of this growth expected to be in the LIB industry. GO and rGO have strong market potentials in various application areas, such as coatings for anticorrosion, anti-icing, and antimicrobial protection, thermal barriers, wear resistance, sensors, additive manufacturing such as 3D inks, and others. GQDs are the emerging key player in the bioimaging, photovoltaics, and light-emitting diodes (LEDs) applications, with the potential to replace traditional semiconductor quantum dots (SQDs), which are based on metallic systems that are more toxic and more expensive. Biomedical applications of GQDs are becoming more attractive because of low to no toxicity and extremely low cost compared to SQDs. The major challenges for scale-up and commercialization of coal-derived carbon products such as graphene vary from the inherent attributes of graphene itself to reluctance to accept graphene in new manufacturing processes because of the uncertainty of the unknown. The 2D nature of graphene materials with a thickness of one atom presents significant challenges to proper handling/processing, and process scale-up becomes difficult because it requires high-end, expensive equipment, even for routine handling and analysis for quality assurance and control. Pristine graphene can also be extremely difficult to work into other matrices, thus hindering downstream processibility, especially at large scale. Currently, the cost of graphene and graphene products is still high and presents an economic risk that tends to slow down investment in scaling up emerging technologies. The lack of a standard for graphene materials for quality assurance and quality control poses a great challenge not only for the markets but also for commercialization efforts. A first-look economic feasibility analysis of the UCP technology provided valuable information that suggests the UCP process would be feasible, especially when it is scaled to a pilot scale and could be more competitive at the full scale. Graphitization was found to be the most energy-consuming and most capital-intensive step in the overall process. In small laboratory- and bench-scale experiments, labor is a significant contributor to the total process costs. Although these energy, capital, and labor constraints contribute to a higher selling price for the product, a preliminary economic model suggests that the process would be feasible at large scale when the process is fully integrated, optimized, and automated.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2021

Residual Insoluble Solids Expected from Saltcake Dissolution

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

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗