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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 OSTI2023

Storing Co 2 in Built Infrastructure: Co 2 Carbonation of Precast Concrete Products

The overall objective of the proposed study was to advance the technical understanding of CO 2 incorporation into novel cementitious materials for the development of high value products that provide a net reduction in carbon emissions. This project combined two primary phases of research that addressed technical barriers related to (i) optimizing CO 2 storage capability of cementitious materials, (ii) evaluating and enhancing physical properties of novel carbonated materials, and (iii) assessing the reductions in life cycle CO 2 emissions attributed to CO 2 carbonation of precast cementitious materials. Engineered cementitious composites (ECC) are a class of highly ductile concrete composites that have been shown to be very durable when used in the built environment. CO 2 carbonation of ECC was examined in this study and it was found that precast ECC specimens could sequester up to 35% CO 2 by cement mass after 24 hours of curing at a CO 2 pressure of 0.5 MPa and 23°C and had a strain capacity of 3%. Carbonation conditions were optimized at the bench-scale and then utilized to create full-scale CO 2 -cured ECC railroad ties that were field tested on a train track. Rail ties were selected for this initial assessment of CO 2 storage in precast concrete materials due to the large market for concrete ties in the railroad industry. Although the full-scale rail ties passed all of the required American Railway Engineering and Maintenance-of-Way Association qualifying mechanical tests, on-track testing of the CO 2 -cured ECC rail ties was unsuccessful due to fiber alignment in the ECC the during the rail tie casting process which prevented the material from achieving the expected level of strain capacity. This result highlights the challenge in scaling up bench-scale processes to full-scale product manufacturing and requires additional investigation into the casting process of large-scale infrastructure elements using ECC combined with carbonation curing. Life cycle assessment of a CO 2 -cured ECC rail tie versus a traditional concrete rail tie indicates that the ECC tie can have lifecycle carbon savings of between 11% and 51% depending on how much longer its useful lifetime is compared to traditional concrete rail ties. Both carbon and cost savings are driven by a reduction in the need to replace broken rail ties, so the key factor is the extent to which a CO 2 -cured ECC rail tie will have increased lifetime durability compared to alternative rail ties.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2021

Predicting Thermal Excursions During in situ Oxidative Regeneration of Packed Bed Catalytic Fast Pyrolysis Catalyst

Ex situ catalytic fast pyrolysis (CFP) uses a secondary reactor to upgrade biomass pyrolysis vapors to stabilized CFP oils with reduced oxygen content. In one configuration, the secondary reactor is operated as a packed-bed swing reactor system which allows coke-deactivated beds to be decarbonized in situ while other beds remain online for vapor upgrading. In situ decarbonization must be done carefully to avoid irreversible deactivation and/or physical degradation of catalyst pellets. Given that packed bed reactors are well known to have poor heat transfer characteristics, this is a critical issue impacting scaleability and commercial viability of the technology. To predict thermal excursions during regeneration, finite element computational models have been built to assist in scaling up oxidative decarbonization of a Pt/TiO2 CFP catalyst (0.5 mm spheres) from a bench scale packed bed with 100 g of catalyst to a pilot scale packed bed with 2 kg of catalyst and internal cooling tubes. Based on transient measurements of outlet temperature and effluent CO2 concentration, and using an assumed coke profile and activation energy, this paper demonstrates that specific combinations of effective thermal conductivity and wall heat transfer coefficient can fit bench scale oxidative regeneration data equally well. For the upscaled 2 kg bed, four bench-scale “best fit” parameter pairs give different predictions for location and magnitude of thermal excursions, with the maximum computed bed temperature gradients ranging from 30 °C cm-1 to as high as 3000 °C cm-1. The larger the fraction of heat removal by conduction through the cooling tubes, the greater the differences between the parameter pairs. The modelling results presented in this paper cast doubt on the industrial viability of the proposed combination of catalyst, bed and regeneration process, and point to the need for alternate reactor designs. However, there is considerable uncertainly in some of the key model parameters. The reliability of model predictions can be increased by adding more temperature measurements at key bed locations, testing additional variations in process conditions, performing careful bed dissections to determine the true coke profile, and perhaps most importantly, directly measuring the effective thermal conductivity of the catalyst pellets.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

AN ACID BAKING APPROACH TO ENHANCE RARE EARTH ELEMENT RECOVERY FROM BITUMINOUS COAL SOURCES

Rare earth elements (REE) are a group of 17 elements typically classified as light and heavy rare earth elements, which play a crucial role in developing the latest technologies for energy, defense, and medical sectors. Even though REEs have been found in more than 200 minerals, only bastnaesite, monazite and xenotime are commercially exploited for REE extraction. However, the recent exponential increase in REE demand has spurred countries such as the United States into research for the extraction of REEs from secondary sources such as coal, acid mine drainage, and coal ash. Several coal sources (e.g., Fire Clay seam coal) across the United States have been identified to contain elevated concentrations of rare earth elements (>600 ppm), and various researchers have investigated the feasibility of both physical and hydrometallurgical extraction techniques for rare earth concentration and subsequent extraction. However, both physical and direct leaching were concluded to be inefficient for RE beneficiation and extraction due to low recoveries. Alternatively, thermal treatment provides promising means for RE recovery from bituminous coal sources. The positive impact of thermal treatment/calcination was established to be due to the decarbonization and dehydroxylation of the clays, which released entrapped rare earth elements within the dominant minerals and converted them into an acid-soluble form. Nonetheless, the improvement in recovery was limited to the light REEs (LREEs) with an insignificant increase in the heavy REEs (HREE). It was demonstrated that the light and heavy REEs in the material were associated with difficult-to-leach minerals such as monazite, xenotime, and zircon, which were not decomposed by simple calcination due to their high thermal stability. Hence, roasting in the presence of chemicals was necessary to ensure the decomposition of those REE-containing minerals. As such, this study was focused on the acid baking treatment of bituminous coals with an aim to enhance REE recovery, especially HREEs. Based on the presence of REE minerals like monazite and xenotime, three pre-leach treatment methods, i.e., 1) roasting, 2) direct acid baking, and 3) acid baking after roasting were investigated. Roasting tests at 600 ⁰C revealed that the recovery of light REEs (LREEs) was enhanced while the recovery of HREEs remained relatively unaffected. LREE and HREE recovery values of 38.3% and 21.3%, respectively, were achieved using a 50 g/L sulfuric acid solution at 5% solid concentration and a solution temperature of 75 ⁰C for 2 hours. Comparatively, direct acid baking at 250 °C provided substantial increased LREE and HREE recovery values to approximately 49.4% and 53.0%, respectively, using an equivalent acid dosage. Recoveries were maximized to 77.0% and 79.6% for LREE and HREE, respectively, by roasting followed by acid baking. Similar results were obtained from the treatment of a second bituminous coal source. Due to strong correlations between REE and Al recovery values, tests were performed on kaolinite and illite, which were prominent clay minerals within the source coals. These experiments revealed that the REE recovery improvements were likely a result of dehydroxylation of clays and subsequent release and decomposition of REE-bearing minerals such as monazite, xenotime and zircon. Subsequently, a parametric study was conducted to identify the impact of acid baking parameters on rare earth element recovery. The factors investigated using a three-level statistical experimental program were acid baking time, acid solution concentration, baking temperature, and acid solution-to-solids ratio which were found to significantly impact REE and contaminant element (Al, Fe, and Ca) recovery. An increase in baking temperature up to around 250 ⁰C improved the light and heavy REE recovery values by more than 50 absolute percentage points relative to performances achieved when direct leaching. As aforementioned, acid baking was needed to both decompose the clay minerals and liberate the REE minerals, which allowed access for the acid to solubilize the REEs. Acid concentration of the solution used for acid baking was studied as a means of minimizing the amount of acid needed to achieve a target REE recovery. However, thermo-gravimetric and differential scanning calorimetry analysis (TGA-DSC) of sulfuric acid under oxidizing atmosphere revealed that the addition of water decreased the evaporation temperature, which explains the lower REE recovery values obtained when using acid concentrations less than 100%. Using pure sulfuric acid at an acid-to-solid ratio of 0.8:1 resulted in recovery values of around 70% for both LREEs and HREEs. The decomposition reaction time was relatively quick with 65% of the TREEs recovered within the first 10 minutes. Following the identification of optimum operating conditions through the parametric study, a systematic leaching study was carried out to examine the impact of leaching parameters, such as solid-to-liquid (S/L) ratio, temperature, and time, on REE recovery using acid baking conditions of 1:1 acid to solids ratio at 250 °C for 30 minutes. The solid-to-liquid ratio was varied from 1-20% by weight at 25 °C, 50 °C, and 75 °C solution temperatures. The results indicated that reaction time and solution temperature considerably impacted the recovery of heavy and light REEs. Interestingly, LREE recovery reduced from 68% at 5% S/L to 58% at 20%S/L, whereas HREE recovery of 78% remained unaffected. The decrease in the LREE recovery was determined to be due to La and Ce precipitation, likely through isomorphic substitution with calcium in gypsum. The kinetic data indicated that 67% LREE and 77% HREE recovery could be obtained within the first 15 minutes of the reaction, suggesting fast reaction kinetics. Furthermore, raising the solution temperature from 25 °C to 75 °C increased the LREE and HREE recovery from 60% and 32% to 67% and 79%, respectively. The kinetic modeling results demonstrated that the rate-limiting step in the LREE dissolution was diffusion and chemical reaction, whereas the HREE extraction was controlled by only chemical reaction. The leaching study concluded that using 20% S/L at 75 °C for 15 minutes maximized LREE and HREE recovery. The lab-scale precipitation study showed that Fe and Al in solution could be removed at pH 4.5 followed by REE precipitation at pH 6.0 using 6 mol/L NaOH. Finally, the bench-scale data was used to develop a process flowsheet for REE recovery from low-grade bituminous coal sources using acid baking. Finally, based on the proposed flowsheet, a concentrated RE-cake obtained through selective precipitation at pH 6.5 was re-leached using HCl at pH 1.5. The resultant leachate was used to identify the impact of various operating parameters on REE recovery and purity with an aim to maximize REE precipitation efficiency while minimizing the oxalic acid dosage. The operating parameters for this investigation were oxalic acid dosage, iron (III) contamination, solution pH and temperature. The resultant model suggested that oxalic acid dosage and reaction pH are the most significant factors for the REE precipitation efficiency, followed by the interaction of oxalic dosage and Fe concentration. Test results indicated that increasing the oxalic acid concentration from 0g/L to 80g/L improved the REE precipitation efficiency from approximately 4.2% to 95.0%. Furthermore, raising the solution pH from 0.5 to 2.5 considerably enhanced the precipitation efficiency from 0.0% to 98.9%. A solution temperature elevation decreased REE recovery, which indicated an exothermic reaction between REEs and oxalate anions. Finally, a high level of Fe contamination adversely impacted REE precipitation efficiency. The speciation analysis revealed that the dominant iron species in the solution system were Fe-(C₂O₄)₃³⁻, Fe-(C₂O₄)²⁻, and Fe-(C₂O₄)⁺, which consumed the majority of the oxalate anions

rare earth elements, acid baking, high-temperature↗
DOE OSTI2021

Effects of carbon treating on piperazine oxidation in pilot plant testing of PZAS™

From February to June 2019, a pilot plant campaign was run for 2100 h at the National Carbon Capture Center (NCCC) using moderately degraded 5 m PZ with simulated flue gas equivalent to a 0.64 MW natural gas combined cycle. Piperazine with the Advanced Stripper™ (PZAS™) and a baghouse were used, and N 2 sparging was applied at the bottom of the absorber. A carbon bed was activated and showed beneficial effects in removing degradation products and reducing the oxidation rate. The cumulative NH 3 production was 180 mmol/k, indicating a PZ oxidation rate of 0.07 mmol/kg/h (0.3 kg PZ/tonne of CO 2 ). The total formate before turning on the carbon bed was 41 mmol/kg, and the total Fe was 0.1 mmol/kg. Carbon treating reduced NH3 production from 0.1 mmol/kg/h to 0.056 mmol/kg/h after 400 h of operation, reduced the UV-Vis absorbance of the samples at 320 nm, and caused a decrease of dissolved Cr. Bench-scale experiments were performed using the NCCC solvent and the same type of carbon. In bench-scale experiments, the UV-Vis absorbance and the concentration of Fe, Mn, and Cr all decreased. Finally, a linear equilibrium relationship was observed between the UV-Vis absorbance and the carbon loading.

03 NATURAL GAS↗
DOE OSTI2023

Developing a Carbon Negative Biorefinery for Organic Waste Valorization

Production of bio-based chemicals have become increasingly attractive as efforts to meet carbon neutrality goals expand. Diverse organic waste feedstocks can be valorized via arrested anaerobic digestion and chain elongation to produce important key intermediates, such as medium chain carboxylic acids. Our work aims to develop a carbon negative biorefinery that funnels multiple organic waste feedstocks into a chemically consistent stream of carboxylic acids that are then upgraded to exemplary carbon negative products. The pairing of a hydrolysis reactor with a chain elongation reactor will allow each biological step to be optimized to improve the ability to valorize a variety of organic waste streams. Specifically, this work has so far been aimed at screening for potential chain elongating organisms to produce VFAs and MCCAs of interest. Four chain elongating organisms were tested for their chain elongation potential with diverse single and mixed substrates. So far, Megasphaera elsdenii and Actinobacillus succinogenes have been tested to determine potential differences in titer as well as product speciation due to variations in pH. To do this, each organism was tested under 3 different substrate combinations with pH maintained at either 5.5, 6, or 7. With better understanding of their metabolic needs and optimal operating conditions, these chain elongating organisms could provide a valuable option to facilitate the chain elongation necessary to produce precursor molecules. In addition to optimizing the bioconversion steps, downstream processing of carboxylic acids is also a key component for the overall feasibility of the process. Our group previously developed a downstream in-situ product recovery (ISPR) process for continuously recovering bio-based carboxylic acids from fermentation broth. The ISPR includes: (i) a solid-liquid separation as a cell retention device, (ii) a liquid-liquid extraction (LLE) to selectively extract the desired bio-based acids, and (iii) a distillation to obtain the neat product. The integrated process was demonstrated at bench-scale and is now scaled up for pilot-scale operations. A more cost-efficient membrane-based emulsion separation is introduced for LLE in downstream separation process with greatly promoted mass transfer, leading to -2800 times smaller needed membrane area than membrane contactors to achieve the same butyric acid extraction rate.

BIOMASS FUELS↗
DOE OSTI2020

Treatment of Problematic Reactive Metal Wastes Using the GeoMelt{sup R} In-Container Vitrification (ICV{sup TM}) Process - 20326

Decommissioning of sodium-cooled reactors and fast reactor technologies has generated a number of reactive metal waste configurations that are problematic to treat and typically lack cost effective treatment methods and disposition options. As a result, Veolia Nuclear Solutions, under contract with Idaho National Laboratory (owned by the U.S. Department of Energy and managed and operated by Battelle Energy Alliance, LLC) demonstrated its GeoMelt{sup R} In-Container Vitrification (ICV){sup TM} technology to safely convert sodium metal to a non-reactive vitrified oxide form. The demonstration project, supported by glass formulation and crucible testing, consisted of a series of ICV{sup TM} melts that processed elemental sodium into stable non-reactive glass. INL is currently implementing GeoMelt{sup R} technology as a means to safely and reliably convert radioactive reactive metal residues that contaminate sodium cooled reactor components into waste forms that comply with existing disposition pathways. Reactive metal wastes require treatment in order to remove the Resource Conservation and Recovery Act (RCRA) reactivity and ignitability characteristics to comply with land disposal restrictions. GeoMelt{sup R}, which is an alternative to other potential treatment approaches, provides a robust approach that chemically converts the reactive metals to an inert oxide while also immobilizing radionuclides in a vitrified waste form with durability equal to or better than vitrified nuclear fuel reprocessing wastes (very robust and inert waste forms). Most other treatment approaches generate hydrogen gas which is problematic. In 2016, Veolia Nuclear Solutions first demonstrated the effectiveness of the GeoMelt{sup R} ICV{sup TM} process in deactivating reactive sodium metal. Crucible, bench-scale, and engineering-scale demonstrations were conducted on several surrogate waste configurations with various ratios of sodium metal and glass formers. Each ratio and configuration demonstrated complete deactivation of the surrogate sodium metal. Follow-on work in 2017 demonstrated the deactivation of reactive sodium by GeoMelt{sup R} ICV{sup TM} at a higher waste loading relative to previously demonstrated work performed in 2016; the higher waste loading optimized glass chemistry while enhancing the economical full-scale treatment of reactive metals. Additionally, follow-on demonstration testing in 2018 and 2019 focused on more complex shapes and other reactive-metals (mocked up Experimental Breeder Reactor II [EBR-II] subassembly, sodium filled heat exchanger, and a can containing sodium potassium alloy) which were all performed at engineering scale. Veolia Nuclear Solutions designed, installed, and commissioned in September 2018, at Perma-Fix Northwest in Richland Washington, a 10-metric ton full-scale GeoMelt unit (GeoMelt{sup R} Richland) for the treatment of reactive metal wastes. As of September 2019, over 900 55-gallon drums containing a total of around 3,500 lb of sodium with low levels of radioactivity have been treated at GeoMelt{sup R} Richland, with resulting glass monoliths disposed at the Nevada National Security Site (NNSS). A full-scale radiological demonstration melt on an actual EBR-II subassembly has also been performed using the full-scale melter in 2019. The GeoMelt{sup R} technology is a proven radioactive waste treatment technology capable of immobilizing radioactive wastes, including bulk rubble such as drums and other steel vessels usually without pretreatment. Utilizing the GeoMelt{sup R} technology to treat reactive metals eliminates pretreatment steps resulting from having to separate the reactive metal from steel containers or jackets as GeoMelt{sup R} can easily operate at temperatures sufficient to melt the steel and expose the reactive metal for treatment. Eliminating handling steps of reactive metals is a significant safety advantage since reactive metals are pyrophoric. The results generated as a part of the 2018-2019 demonstration program are presented in the paper. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Design and Validation of a High-Throughput Reductive Catalytic Fractionation Method

Reductive catalytic fractionation (RCF) is a promising method to extract and depolymerize lignin from biomass, and bench-scale studies have enabled considerable progress in the past decade. RCF experiments are typically conducted in pressurized batch reactors with volumes ranging between 50 and 1000 mL, limiting the throughput of these experiments to one to six reactions per day for an individual researcher. Here, we report a high-throughput RCF (HTP-RCF) method in which batch RCF reactions are conducted in 1 mL wells machined directly into Hastelloy reactor plates. The plate reactors can seal high pressures produced by organic solvents by vertically stacking multiple reactor plates, leading to a compact and modular system capable of performing 240 reactions per experiment. Using this setup, we screened solvent mixtures and catalyst loadings for hydrogen-free RCF using 50 mg poplar and 0.5 mL reaction solvent. The system of 1:1 isopropanol/methanol showed optimal monomer yields and selectivity to 4-propyl substituted monomers, and validation reactions using 75 mL batch reactors produced identical monomer yields. To accommodate the low material loadings, we then developed a workup procedure for parallel filtration, washing, and drying of samples and a 1H nuclear magnetic resonance spectroscopy method to measure the RCF oil yield without performing liquid-liquid extraction. As a demonstration of this experimental pipeline, 50 unique switchgrass samples were screened in RCF reactions in the HTP-RCF system, revealing a wide range of monomer yields (21-36%), S/G ratios (0.41-0.93), and oil yields (40-75%). These results were successfully validated by repeating RCF reactions in 75 mL batch reactors for a subset of samples. We anticipate that this approach can be used to rapidly screen substrates, catalysts, and reaction conditions in high-pressure batch reactions with higher throughput than standard batch reactors.

BIOMASS FUELS,INORGANIC, ORGANIC, PHYSICAL, AND AN↗
DOE OSTI2022

Purification of Degraded Aqueous Piperazine by Ion Exchange and Carbon Treating

Amine purification by ion exchange and carbon treating has been performed for decades to maintain low solvent impurity levels in amines used in natural gas sweetening. The use of these purification methods to remove dissolved metal catalysts and other impurities from amines used in post-combustion carbon capture is less well known. This report presents batch experiments testing the equilibrium adsorption of impurities from degraded piperazine (PZ) onto activated carbon and various ion exchange resins. Compared to cationic exchange, anionic exchange was found to better remove catalytic Fe and UV active species, making it a better candidate for large-scale PZ purification. Carbon treating greatly outperforms anion exchange in the removal of UV active species, but the adsorbents’ difference is less pronounced for the removal of other impurities. Equilibrium adsorption was determined by the UV absorption of the PZ solution at 320 nm, and the results will show this may not be an accurate way to determine equilibrium. Further bench-scale experiments comparing ion exchange and carbon treating are necessary before advancing to larger-scale testing.

amine purification↗
DOE OSTI2023

Small Business Voucher Program: Scaling-Up of Bio-Based C5 Building Block Production: Cooperative Research and Development Final Report, CRADA Number CRD-16-00611

Visolis, Inc. is an early stage industrial biotechnology company developing next generation of processes for producing building blocks for bulk polymers and fuels. The company is developing low-cost routes to the chemicals of the future in support of DOE, EERE and BETO goals to grow the U.S. bioeconomy. NREL has capabilities in scale-up of fermentation processes from bench top through pilot scales and also has expertise and technologies related to production of lignocellulosic sugars from cellulosic feedstocks. NREL's Integrated Biorefinery Research Facility (IBRF) houses multiple fermentation vessels/systems ranging in size from 0.5 to 9,000 L along with ancillary capabilities in compositional analysis, separations, and purification. NREL's role will be to scale-up the Visolis process to produce an intermediate product, mevalonic acid, from both dextrose and biomass derived sugars. The goals of the project are to: 1) transfer and reproduce one of Visolis's proprietary fermentation processes at bench top and pilot scale at NREL's IBRF using dextrose as the feedstock, 2) carry out bench-scale fermentations using Visolis's organism and cellulosic sugars, and 3) produce mevalonic acid from the bench top and pilot scale runs for catalyst lifetime testing and conversion to isoprene.

09 BIOMASS FUELS↗
DOE OSTI2021

A Scalable Process for Upcycling Carbon Dioxide (CO 2 ) and Coal Combustion Residues into Construction Products

Anthropogenic sources of carbon dioxide are generated from a number of sources, but the key among these are ordinary Portland cement (OPC) production and combustion of fossil fuels. Cement production is the largest global CO 2 source from the mineral decomposition of carbonates. Combination of the limestone decomposition and thermal requirements of the clinkering process causes cement production to contribute 8-9% of annual global CO 2 emissions. Combustion of fossil fuels (coal, oil and gas) was shown to contribute a much larger portion of global CO 2 emissions. As of 2018, combustion of fossil fuels accounted for 65% of global CO 2 , where 41% was derived from stationary sources for electricity and heat generation and the other 24% was related to transport. To reduce these contributions, key steps forward in CO 2 utilization technologies are required. The purpose of this project is to demonstrate the feasibility of the Reversa process evolving from a TRL-3 technology at the bench-scale up to TRL-6 technology at the pilot-scale. The reliability of the Reversa technology was tested to prove the effective production of concrete masonry units (CMUs) at bench scale, where the units exceeded the required 13.8 MPa compressive strength requirements. The overall goal of this project was to accelerate the development of a CO 2 mineralization process that synergistically utilizes CO 2 in flue gas and coal combustion residues (CCRs) to synthesize carbonated concrete, a functional replacement for traditional concrete. The culmination of this work resulted in 12 successful production runs at the Integrated Test Center (ITC), Gillette, WY using coal flue gas as a CO 2 source. This was followed by 6 production runs which were completed at the National Carbon Capture Center (NCCC), Wilsonville, AL, using coal-fired and natural gas (NG) flue gas as the CO 2 source. Over the course of the production runs at NCCC and ITC, the CO 2 utilization as a function of time, 24-h CO 2 uptake, electricity usage, and 28-d net area compressive strength recorded for each run. The ITC and NCCC demonstrations achieved an average of 0.19 and 0.1 g CO 2 /g reactant, respectively. Both demonstrations exceeded the project’s target goals of uptake > 0.05 g CO 2 /g reactant. Average compressive strength of the ITC blocks was 18.24 MPa at 28-days. This exceeded the target strength of 13.8 MPa specified by ASTM C90. ITC and NCCC produced an average CO 2 utilization efficiency of 74.9 and 57.9%, respectively. Both demonstration averages were within the target range of 50 to 90% utilization efficiency. For some production runs the NCCC demo did exceeded the a CO 2 utilization efficiency of 75%. An LCA of the Reversa process compared to an industry standard product revealed a net CO 2 reduction of 39% to 42%. This exceeded the target requirement of >25% net CO 2 reduction. Collection of this data was used to determine that the project was successful as the demonstration goals were achieved: (1) achieving in excess of 75% CO 2 utilization efficiency, (2) utilizing greater than 250 kg of CO 2 per production batch/run, and (3) ensuring compliance of carbonated blocks with industry standard specifications (ASTM C90).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Developing novel electrodes with ultralow catalyst loading for high-efficiency hydrogen production in proton exchange membrane electrolyzer cells

Hydrogen plays more crucial roles for decarbonizing the planets and meeting the climate challenges because of its high energy density and zero-emission. It can be produced with proton exchange membrane electrolyzer cells (PEMECs) driven by sustainable and renewable energy resources. Although PEMECs have a number of advantages, including high purity production, quick response, and the ability to operate at high pressure facilitating the gas delivering, their performance and cost greatly hinder their commercial-scale applications. To achieve high-efficiency and cost-reduced hydrogen production in PEMECs, we proposed thin engineered liquid/gas diffusion layers (LGDLs) and associated electrodes, i.e., catalyst-coated LGDLs (CCLGDLs), over conventional porous transport layers (PTLs) and catalyst-coated membranes (CCMs). The research approaches in this project are based on material synthesis, in-situ and ex-situ characterizations, component design and treatment, numerical modeling, and cost analysis. The thin and tunable LGDLs (TT-LGDLs) and CCLGDLs were successfully developed with great performance improvement as demonstrated in lab-scale, bench-scale, and system-scale electrolyzer tests. The electrode thickness was reduced from 370 µm to less than 100 µm with simplified fabrication processes. With the catalytically enhanced Ir-based catalyst coating, the as-developed CCLGDLs with a catalyst loading of 0.34 mg Ir /cm 2 achieved a cell performance of 1.77 V at 2 A cm -2 , exhibiting the catalyst mass activity enhanced by >20 times with significant catalyst saving over conventional catalyst cell design. In-situ PEMEC characterizations, including the current distribution mapping and high-speed and multiscale visualizations, were conducted for a deeper understanding of mass transport and electrochemical reactions within an electrolyzer with LGDLs and CCLGDLs. A 2D cell model was developed and validated for the enhanced performance on TT-LGDL through reducing ohmic losses due to nonuniform hydration and water transport. Further, the cost analysis results have shown a path to move beyond equivalency and surpass costs associated with the project baseline. In this project, the design and fabrication of TT-LGDLs and CCLGDLs will contribute to the performance enhancement, manufacturing simplification, and cost reduction for PEMECs and other energy conversion devices, thus shortening their pathways towards commercialization. This project also provides a good foundation for furthering the in-situ reaction interface research.

08 HYDROGEN↗
DOE OSTI2022

Removal of Tc-99, Zr-95, and Nb-95, From Solutions Obtained After Dissolution of Irradiated Mo Targets

Decontamination of 99 Tc, Nb, and Zr impurities in dissolved irradiated Mo disks can be accomplished using Fe(II) precipitation. Here, we report bench-scale experiments and large-scale demonstrations on removal of 99 Tc (0.1 mM), 95 Nb, and 95 Zr from dissolved Mo disk simulant solutions. Tc removal is accomplished through the reduction and simultaneous immobilization of Tc(VII) by Fe(II), producing an insoluble, Tcincorporated Fe(II)-Fe(III) solid that is removed by filtration. Large-scale testing showed that Tc (97.6% ± 1.7%) is removed without affecting 99 Mo yields. Other important side reaction product impurities in irradiated Mo targets, namely various isotopes of Nb and Zr, are also removed (>99%) in this process. The effects of metal (Fe, Tc, Mo) concentrations, Fe(II)/Fe(III) ratio, pH, temperature, Fe addition method, and hydrogen peroxide addition were tested. The minimum amount of Fe(II) needed to remove up to 99% Tc is 10 mM and the optimal pH value for simultaneous removal of Tc, Nb, and Zr impurities is pH 13.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Integrated Capture and Conversion of CO 2 to Methanol (ICCCM) Process Technology - CRADA 449 (Final Report)

The goal of this project is to develop a prototype system that integrates the capture and catalytic hydrogenation of CO 2 into methanol in the same solvent. Ultimately, this integrated approach could provide a technology with projected reductions to capital and operating costs by at least 20% relative to a benchmark methanol synthesis via gas-phase CO 2 hydrogenation. There were five primary objectives for the project: 1. Optimize the selections of both the catalysts and the CO 2 capture solvents to achieve high conversion (>80%) and high selectivity (>90%) toward methanol in the targeted processing ranges (100-180°C, 1-60 bar). 2. Design a reactor system that provides a fixed catalyst surface area and high-efficiency heat exchange to assure compact modular processing. 3. Build and test a reactor system and demonstrate in a bench scale continuous flow system, and use the operating data to refine the comparison to existing conversion technologies. 4. Refine techno economic (TEA) and Tech-to-Market (TTM) analyses using the experimental data obtained from the bench-scale system. 5. Use the experimental data and TEA/TTM projections to develop a conceptual design for a pre-commercial system that targets a specific market opportunity.

09 BIOMASS FUELS↗
DOE OSTI2022

A Novel Process for Carbon Dioxide Conversion to Fuel

In this project, TDA developed a new mixed metal oxide-based sorbent that converts CO2 (captured from coal fired power plants) to CO, which can then be combined with renewable H2 generated by water electrolysis or H2 from steam methane reforming to produce different liquid fuels. TDA’s absorbent-based CO2 conversion process uses a redox process, which splits the catalytic reforming of methane with CO2 reaction into two stages: CO2 reduction to CO and CH4 reforming into H2 and CO which eliminates the equilibrium limitations. The CO produced in the two-stage reactor system can then be further reacted with renewable H2 to produce methanol, naphtha, diesel, or gasoline. We worked with the Advanced Power & Energy Program (APEP) of University of California, Irvine (UCI) to design and develop the liquid fuel synthesis process that is built around this new material. We demonstrated the techno-economic viability of the new sorbent based redox process to convert CO2 into synthesis gas by demonstrating continuous carbon dioxide reduction in a prototype test system for over 585 hours while converting up to 10 kg CO2/day. With the successful completion of the R&D effort, the technology is now ready for a larger pilot-scale demonstration and the technology readiness has been raised from TRL 3 to TRL 5. In collaboration with UCI, we completed a high-fidelity process design and economic analysis. The required sale price (RSP) for gasoline (Case 1 NG-MTG) is $4.91/gal and naphtha and diesel (Case 2 NG-FT) are $4.23/gal and $6.07/gal, respectively, on a 2011 dollar basis. To put these costs in perspective, the California prices in current dollars (with its strict specifications) for regular grade gasoline from last year to current year have varied from a low of $3.10/gal in January 2021 to a high of $5.76/gal in March 2022, while prices for diesel from last year to current year have varied from a low of $3.40/gal in January 2021 to a high of $6.41/gal in May 2022 according to the U.S. Energy Information Agency data. It should be noted that the gasoline and diesel produced by these designs of Case 1 and Case 2 would be of very high quality and both nitrogen and sulfur free. These RSPs are based on a cost of imported electricity of $64/MWh based on the low-end current wind generated electricity cost (Genevieve 2011). This cost is by far the largest component of the variable costs used in computing the RSPs. A sensitivity analysis of these RSPs to the cost of imported electricity shows that the cost of the imported electricity has a significant effect on the RSPs. The life cycle analysis (LCA) shows that the total cradle-to-gate CO2 emissions for both liquid fuels (diesel and gasoline) were negative, indicating that overall more CO2 is consumed than released during production of the fuel from CO2 feed stack for both cases (-296 kgCO2 per MT gasoline for Case 1 and -705 kgCO2 per MT diesel for Case 2). On a cradle-to-grave comparison, the use of diesel produced using TDA’s process (2,457 kgCO2 per MT diesel) would release 37.6% less CO2 compared to petroleum based diesel (3,937 kgCO2 per MT diesel) while the use of gasoline produced using TDA’s process (2,792 kgCO2 per MT gasoline) would release 29.3% less CO2 compared to petroleum based gasoline (3,946 kgCO2 per MT gasoline). With the successful completion of the R&D effort, the technology is now ready for a bench-scale demonstration and the technology readiness has been raised from TRL 3 (Analytical and experimental critical function and/or characteristic proof of concept) to TRL 5 (Laboratory scale similar system validation in relevant environment).

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2024

Beneficial Use of Harvested Ponded Fly Ash and Landfilled FGD Materials for High-Volume Surface Mine Reclamation

The overall motivation of this project was to demonstrate at laboratory, bench-scale, and full-scale demonstration levels that (a) coal ash surface impoundments can go through closure by removal as per USEPA and state regulations so that the material can be used as is (other than draining free water using CCRs piles) in high-volume beneficial applications, (b) FGD material from closed out FGD facilities can be excavated and recompacted for coal mine reclamation, and (c) harvested CCRs can be beneficially utilized (providing a net environmental gain) in large-volumes for reclamation at abandoned coal mine sites across the US, especially in the Eastern and Midwest coal mining regions. The objectives of this project were to: 1) promote the safe and cost-effective closure by removal of coal ash impoundments, 2) harvest landfilled FGD, and 3) promote the high-volume beneficial use of these harvested CCRs in the reclamation of abandoned surface coal mine sites across the eastern and midwestern coal mining regions of the United States. The major tasks carried out for this project are summarized below: 1) Conesville Full-Scale Demonstration Project: About 2 million tons of harvested CCR materials from the closure by removal of an inactive fly ash pond and an adjacent old FGD landfill were used for the full-scale demonstration project to fully reclaim a nearby partially completed abandoned surface coal mine. Site monitoring for the project duration was carried out and results are discussed. 2) Laboratory Testing: Geotechnical and environmental testing of harvested ponded fly ash and landfilled FGD material at the former Conesville power plant were carried out. Completing the laboratory testing allowed for QA/QC for the full-scale site construction and informed the formulation of the risk analysis. 3) Risk Analysis: We developed a reliable computational model for fate and transport. We used these models and the rich set of monitored data for the Conesville site to analyze risks to human health and ecological risks associated with high-volume surface mine reclamation using harvested CCRs. 4) GIS Siting Study: A Geographic Information System (GIS) study was carried out for three states in the Eastern coal mining region and two states in the Midwest coal region. This effort provided site specific GIS information for five states and allowed us to establish protocols that other states can follow in implementing their own state specific GIS study.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2025

ROTA-CAP™: An Intensified Carbon Capture System Using Rotating Packed Beds (Final Scientific/Technical Report)

GTI Energy and Carbon Clean Solutions Limited successfully designed, constructed, and operated an integrated ROTA-CAP carbon capture skid. ROTA-CAP™ is a process intensification technology, applied for post-combustion carbon capture, which utilizes the centrifugal forces generated from rotation of rotating packed beds as well as advanced solvents to achieve increased mass transfer rates 1-2 orders of magnitude higher than conventional columns while substantially decreasing footprint. The test skid, which consisted of a dual stage RPB absorber with external interstage cooling and a single stage RPB regenerator, was operated at capacities up to 0.5 tonne/day of CO 2 capture with flue gas concentrations ranging from 4% to 22% CO 2 by vol. CO 2 removal rates greater than 95% were achieved, with CO 2 product purity also exceeding 95% by vol. Over 1,600 hours of operation were accumulated throughout the project, including over 1,000 hours of operation of the with real flue gas containing at least 9.8% CO 2 by vol. The skid was operated continuously for 24 hours per day and 7 days per week over the course of 7 long-term test campaigns, with the campaigns ranging from approximately 2-4 weeks per campaign. A techno-economic analysis was performed, and a cost of capture of $\$$41.18/tonne CO 2 was calculated for the ROTA-CAP process, compared to $\$$45.75/tonne for a Cansolv-based process. These results show a cost reduction of approximately 10% compared to the Cansolv-based process. Although this still exceeds the target cost of capture of $\$$30/tonne specified for this project, GTI expects that the cost of capture can be further reduced through further optimization of the design and technology. GTI also performed an engineering design review to determine the scale-up potential of the technology, with the results of the preliminary assessment indicating that it appears to be feasible to scale up the RPB technology to 4,000 TPD. It was also determined that both horizontal and vertical rotor orientations are feasible, though there are mechanical advantages to the vertical orientation.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2024

Achieving Unprecedented CO 2 Utilization InCO 2 Concrete™: System Design, Product Development and Process Demonstration

Anthropogenic sources of carbon dioxide are generated from a number of sources, but the key among these are ordinary Portland cement (OPC) production and combustion of fossil fuels. Cement production is the largest global CO 2 source from the mineral decomposition of carbonates. This is due to the clinkering process whereby limestone (mainly consisting of CaCO 3 ) is decomposed into CaO and CO 2 , and combined with silica rich clays at high temperatures to form clinkers (i.e. the four key minerals that comprise cement). The high temperature range of 1400 – 1550°C required for this process accounts for up to 60% of the generated CO 2 from cement production. Combination of the limestone decomposition and thermal requirements of the clinkering process causes cement production to contribute 8-9% of annual global CO 2 emissions. Combustion of fossil fuels (coal, oil and gas) was shown to contribute a much larger portion of global CO 2 emissions. As of 2018, combustion of fossil fuels accounted for 65% of global CO 2 , where 41% was derived from stationary sources for electricity and heat generation and the other 24% was related to transport. To reduce these contributions, key steps forward in CO 2 utilization technologies are required. Therefore, a CO 2 mineralization technology (CO 2 mineralization concrete) to reduce the OPC content in concrete, while utilizing flue gas emissions from fossil fuel combustion has been developed to address both areas simultaneously. This Reversa™ technology utilizes low-carbon cementation agents produced by in situ CO 2 mineralization (“mineral carbonation reactions”) to offer a promising alternative to OPC. CO 2 mineralization relies upon the reaction of dissolved CO 2 with inorganic alkaline reactants to precipitate mineral carbonates (e.g., CaCO 3 ), which bind proximate particles and achieve cementation. Herein, a concrete green body, which is composed of a mixture of binder, water, and mineral aggregates, is exposed to CO 2 borne in industrial flue gas streams. This manner of CO 2 mineralization allows the production of construction components that feature equivalent engineering attributes as their OPC-based counterparts while featuring a much smaller embodied carbon intensity (eCI). The purpose of this project is to demonstrate the feasibility of the Reversa process evolving from a TRL-3 technology at the bench-scale up to TRL-6 technology at the pilot-scale. The reliability of the Reversa technology was tested to prove the effective production of three standard industrial concrete products selected during the course of the project. The results detailed herein will demonstrate the evolution of this technology to the industrial scale. The culmination of this work resulted in 9 production runs completed at the National Carbon Capture Center (NCCC), Wilsonville, AL, using natural gas (NG) flue gas as the CO 2 source. Over the course of the production runs at NCCC, the CO 2 utilization as a function of time, 24-h CO 2 uptake, electricity usage, and 28-d net area compressive strength recorded for each run. Collection of this data will be used to determine the success of the demonstration goals: (1) achieving in excess of 0.2gCO 2 /g reactant , (2) achieving greater than 50% reduction in global warming potential compared to standard produced units, and (3) ensuring compliance of carbonated concrete with industry standard specifications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Bench-Scale Development of Promoted High-Capacity Structured Sorbents (Final Technical Report)

The project objective was to develop high-capacity structured sorbent capable of achieving low CO 2 removal from air. The sorbent framework consists of an amine-functionalized onto hydrophobic polymer backbone with an added promoter. The functionalized amine provides high CO 2 capacity and adsorption rates and the polymer backbone to reduce water uptake. For the sorbent development, multiple functionalized amines and promoters were assessed to select a candidate that achieved high CO 2 capacity, high adsorption rate, and high stability. A sorbent-coated filter design was selected as the structured sorbent, which provides high sorbent loading capacity and contains an electrically conductive nonwoven filter substrate that can be Joule-heated to provide efficient utilization of available electricity for sorbent regeneration. A commercial partner operated a pilot filter manufacturing line to produce the filter panels coated with the developed sorbent. A 1 kg CO 2 /day bench unit was designed and fabricated to test the structured filter sorbent. The key achievements from the structured sorbent development activity were demonstrating that existing filter industrial-scale processes can be used for manufacturing Susteon’s structured sorbent and completing a proof-of-concept demonstration of the commercially manufactured structured sorbent filters for CO 2 capture from air with direct, Joule-heated regeneration. A techno-economic assessment with sensitivity analysis was conducted on a 100,000 TPY facility with 85% operating capacity. Through sorbent optimization and process design improvements, it is estimated that the cost of capture was reduced from $\$$349/tCO 2 to $\$$241/tCO 2 . The TEA projects further reductions to $165/tCO 2 through enhancements in CO 2 adsorption rate and sorbent capacity and reducing manufacturing and scale up risks. A life cycle analysis was conducted on the same 100,000 TPY facility and confirmed that the facility’s electricity demand drives its greenhouse gas impact. It was determined that electricity supplied through the current grid mix would result in net-positive CO 2 emissions and that achieving net-negative emissions is only possible by powering the system with renewable electricity or fossil fuel sources equipped with carbon capture and sequestration.

36 MATERIALS SCIENCE↗