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DOE OSTI2022

M2CT-22IN1202096 Design for Carbon Conversion Product Pathways with Nuclear Power Plant Integration

Coal is a globally abundant resource that historically has been used for power generation via combustion. As the power industry replaces coal with cleaner methods of generation, energy-rich coal could be used in other chemical and fuel applications. This study presents a coal utilization option in which coal combustion is replaced with a carbon-free nuclear power plant and the coal is upgraded to valuable products for a variety of markets. Coal is prepared for conversion first by the pyrolysis process, which will optimize solid, liquid, and gaseous products based on the market size and potential product value, maximizing the monetary value of coal. This process is designed using bituminous coal from the Appalachian region as a basis to provide a pathway to preserve or transition coal-related jobs and create new jobs associated with the clean energy transition. Process modeling in the AspenOne Suite will be used to determine each component’s sensitivities, costs, inputs, and outputs. Dispatch modeling in the FORCE toolset will optimize the entire system and calculate the NPV for the refinery lifetime. Advanced and light-water reactors are considerations to supply the heat, steam, and electricity to the process. This paper focuses on the technical and market analysis used to determine the optimal processes and product pathways for the carbon refinery. Product pathways are on activated carbon, formic acid synthesis, and methanol synthesis for further upgrading to marketable chemical and polymer products.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2022

Design for Carbon Conversion Product Pathways with Nuclear Power Plant Integration (PCC)

Coal is a globally abundant resource that historically has been used for power generation via combustion. As the power industry replaces coal with cleaner methods of generation, energy rich coal could be used in other chemical and fuel applications. This study presents a coal utilization option in which coal combustion is replaced with a carbon-free nuclear power plant and the coal is upgraded to valuable products for a variety of markets. Coal is prepared for conversion first by the pyrolysis process, which will optimize solid, liquid, and gaseous products based on the market size and potential product value, maximizing the monetary value of coal. This process is designed using bituminous coal from the Appalachian region as a basis to provide a pathway to preserve or transition coal-related jobs and create new jobs associated with the clean energy transition. Process modeling will be used to determine each component’s sensitivities, costs, inputs, and outputs Advanced and light-water reactors are considerations to supply the heat, steam, and electricity to the process. This paper focuses on the technical and market analysis used to determine the optimal processes and product pathways for the carbon refinery. Product pathways are on activated carbon, formic acid synthesis, and methanol synthesis for further upgrading to marketable chemical and polymer products.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2025

EM Physics

Geant4 provides a comprehensive set of electromagnetic (EM) processes and models for electron/positron, gamma and long-lived charged particles, spanning energies from 100 eV to 100 TeV. Covering diverse energy regions often requires multiple models, which can be constructed using pre-packaged or user-defined EM physics constructors. Geant4 also supports detailed low-energy EM physics through models like Livermore, Penelope, and ICRU73, offering extensive data for elements across a wide energy range (250 eV–100 GeV). Application domains include space, medical, and radiobiology simulations. Additionally, Geant4 provides robust options for simulating complex optical photon production and transportation processes, enhancing its versatility in physics research and applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Nanowire-based hydrodesulfurization catalysts for hydrocarbon fuels

The present development is a metal particle coated nanowire catalyst for use in the hydrodesulfurization of fuels and a process for the production of the catalyst. The catalyst comprises titanium(IV) oxide nanowires wherein the nanowires are produced by exposure of a TiO2—KOH paste to microwave radiation. Metal particles selected from the group consisting of molybdenum, nickel, cobalt, tungsten, or a combination thereof, are impregnated on the metal oxide nanowire surface. The metal impregnated nanowires are sulfided to produce catalytically-active metal particles on the surface of the nanowires The catalysts of the present invention are intended for use in the removal of thiophenic sulfur from liquid fuels through a hydrodesulfurization (HDS) process in a fixed bed reactor. The presence of nanowires improves the HDS activity and reduces the sintering effect, therefore, the sulfur removal efficiency increases.

Sunkara, Mahendra Kumar↗

DOE OSTI2022

Nanowire-based hydrodesulfurization catalysts for hydrocarbon fuels

Sunkara, Mahendra K.↗

DOE OSTI2025

Metallurgical Analysis and Forward Modeling of Weld Distortion in SMR Containment Vessels

This work aimed to apply Sandia’s expertise in metallurgy and modeling to enable the use of hybrid laser arc welding for building nuclear reactor containment structures, via a collaboration with Holtec International. Experimental observations were coupled with finite element analysis to resolve microstructure development, mechanical properties, distortion, and residual stress in welds relevant to the production of the Holtec SMR-160. High residual stresses were observed in welds that were not subjected to preheat. Meanwhile, the microstructure of the welds generally exhibited a narrow heat affected zone relative to conventional arc welds. FEA appeared to be effective in simulating the thermal/mechanical conditions that occur during hybrid laser arc welding of simplified and instrumented test welds. Subsequently, FEA was used to perform sensitivity analyses for various weld geometries that would be prohibitively costly to assess with physical experiments. Insights from the study were used to inform Holtec’s welding process, and successful production welds were performed in 2025.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2021

Halophyte biorefinery for polyhydroxyalkanoates production from Ulva sp. Hydrolysate with Haloferax mediterranei in pneumatically agitated bioreactors and ultrasound harvesting

Here, the present study tested the outdoor cultivation of Haloferax mediterranei for PHA production from green macroalgae Ulva sp. in pneumatically agitated bioreactors and applied ultrasonic separation for enhanced settling of archaeal cells. Scaled-up cultivation (40 L) yielded maximum biomass productivity of 50.1 ± 0.11 mg·L -1 ·h -1 with a PHA productivity of 27 ± 0.01 mg·L -1 ·h -1 and conversion yield of 0.107 g PHA per gram UlvaDW. The maximum mass fraction of PHA achieved in biomass was calculated to be 56% w/w. Ultrasonic harvesting of Hfx. mediterranei cells approached 30% removal at energy inputs around 7.8 kWh·m -3 , and indicated no significant aggregation enhancement by Ca 2+ addition. Molecular weight analysis showed an increase in Polydispersity Index (PDI) when the corresponding air velocities were increased suggesting that the polymer was more homogeneous at lower mixing velocities. The current study demonstrated scalable processes for PHA production using Ulva sp. feedstock providing new technologies for halophilic biorefinery.

09 BIOMASS FUELS↗

DOE OSTI2022

Glass Property-Composition Models for Support of Hanford WTP LAW Facility Operation

Current plans for the River Protection Project envision starting to vitrifying low-activity waste (LAW) by 2023 using a Direct Feed Low-Activity Waste (DFLAW) approach and subsequently using a full-pretreatment approach. The Hanford Tank Waste Treatment and Immobilization Plant (WTP) LAW Facility will be operated and controlled using a LAW glass formulation algorithm (GFA), which requires several inputs based on research and development results. LAW glass property-composition models for several product quality and processing properties are key inputs for the LAW GFA. It is envisioned that the preliminary LAW GFA discussed by Kim and Vienna (2012) will be used for commissioning and initial radioactive operations of the WTP LAW Facility under Bechtel National, Inc. using the DFLAW approach. Then, an updated LAW GFA will be developed for implementation by the WTP operating contractor that takes over after WTP LAW Facility commissioning. This report documents the enhanced LAW glass property-composition models developed for use in the updated LAW GFA. The properties for which models were developed include Product Consistency Test (PCT) response, Vapor Hydration Test (VHT) response, viscosity at 1150 °C, electrical conductivity at 1150 °C, melter SO 3 tolerance at 1150 °C, and K-3 refractory corrosion at 1208 °C. Table S.1 lists the tables in this report that contain the recommended models for each of these properties. The model types recommended include partial quadratic mixture (PQM) models for viscosity, electrical conductivity, melter SO 3 tolerance and K-3 corrosion, bias corrected PQM model (bcPQM) for PCT, and logistic PQM model for VHT. The fits of model and validation subsets were found to be well predicted by the recommended models.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Glass Property-Composition Models for Support of Hanford WTP LAW Facility Operation

Current plans for the River Protection Project envision starting to vitrifying low-activity waste (LAW) by 2023 using a Direct Feed Low-Activity Waste (DFLAW) approach and subsequently using a full-pretreatment approach. The Hanford Tank Waste Treatment and Immobilization Plant (WTP) LAW Facility will be operated and controlled using a LAW glass formulation algorithm (GFA), which requires several inputs based on research and development results. LAW glass property-composition models for several product quality and processing properties are key inputs for the LAW GFA. It is envisioned that the preliminary LAW GFA discussed by Kim and Vienna (2012) will be used for commissioning and initial radioactive operations of the WTP LAW Facility under Bechtel National, Inc. using the DFLAW approach. Then, an updated LAW GFA will be developed for implementation by the WTP operating contractor that takes over after WTP LAW Facility commissioning. This report documents the enhanced LAW glass property-composition models developed for use in the updated LAW GFA. The properties for which models were developed include Product Consistency Test (PCT) response, Vapor Hydration Test (VHT) response, viscosity at 1150 °C, electrical conductivity at 1150 °C, melter SO3 tolerance at 1150 °C, and K-3 refractory corrosion at 1208 °C. Table S.1 lists the tables in this report that contain the recommended models for each of these properties. The model types recommended include partial quadratic mixture (PQM) models for viscosity, electrical conductivity, melter SO 3 tolerance and K-3 corrosion, bias corrected PQM model (bcPQM) for PCT, and logistic PQM model for VHT. The fits of model and validation subsets were found to be well predicted by the recommended models.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

Self-Buffering system for Cost-Effective production of lactic acid from glucose and xylose using Acid-Tolerant Issatchenkia orientalis

This study presents a cost-effective strategy for producing organic acids from glucose and xylose using the acid- tolerant yeast, Issatchenkia orientalis. I. orientalis was engineered to produce lactic acid from xylose, and the resulting strain, SD108XL, successfully converted sorghum hydrolysates into lactic acid. In order to enable low- pH fermentation, a self-buffering strategy, where the lactic acid generated by the SD108XL strain during fermentation served as a buffer, was developed. As a result, the SD108 strain produced 67 g/L of lactic acid from 73 g/L of glucose and 40 g/L of xylose, simulating a sugar composition of sorghum biomass hydrolysates. Moreover, techno-economic analysis underscored the efficiency of the self-buffering strategy in streamlining the downstream process, thereby reducing production costs. These results demonstrate the potential of I. orientalis as a platform strain for the cost-effective production of organic acids from cellulosic hydrolysates.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Data for Self-Buffering System for Cost-Effective Production of Lactic Acid from Glucose and Xylose Using Acid-Tolerant Issatchenkia orientalis

This study presents a cost-effective strategy for producing organic acids from glucose and xylose using the acid-tolerant yeast, Issatchenkia orientalis . I. orientalis was engineered to produce lactic acid from xylose, and the resulting strain, SD108XL, successfully converted sorghum hydrolysates into lactic acid. In order to enable low-pH fermentation, a self-buffering strategy, where the lactic acid generated by the SD108XL strain during fermentation served as a buffer, was developed. As a result, the SD108 strain produced 67 g/L of lactic acid from 73 g/L of glucose and 40 g/L of xylose, simulating a sugar composition of sorghum biomass hydrolysates. Moreover, techno-economic analysis underscored the efficiency of the self-buffering strategy in streamlining the downstream process, thereby reducing production costs. These results demonstrate the potential of I. orientalis as a platform strain for the cost-effective production of organic acids from cellulosic hydrolysates.

Conversion↗

DOE OSTI2023

Behavioral simulations and experimental evaluations of stress induced spatial nonuniformity of dynamic bulk modulus in additive friction stir deposited AA 6061

Additive friction stir deposition (AFSD) is a rapidly developing solid-state additive manufacturing (AM) technology that enables the fabrication of customized products on a relatively large scale. The unique forge-liked process offers high quality products with refined equiaxed microstructure and exceptional mechanical performance. However, in AFSD, the spatially distributed mechanical properties within a deposited layer have not been established so far, due to the lack of a suitable large-scale mapping method. In the present work, an ultrasonic dynamic-elasticity mapping method was employed to map the distribution of physical properties in a AFSD 6061 Al. Strong spatial asymmetries in elastographies were mainly due to the residual stresses. The origin of the asymmetries was investigated through thermo-mechanical simulations of the AFSD process. It was observed that majority of the asymmetries were associated with the mechanical residual stresses instead of the symmetric thermal residual stresses during linear deposition of the AFSD process. However, the thermal residual stresses can be manipulated to become asymmetric with a 90° turn in the linear deposition path, due to the difference between the levels of cooling along the edges of the inner and outer corners. Hence, the mechanical and thermo-mechanical residual stresses can be additive or subtractive depending on the direction of the turns. Here, such numerically predicted behaviors were also experimentally observed on the AFSD fabricated samples by ultrasonic elastography. Furthermore, additional preliminary studies on multi-layer AFSD fabrications show the asymmetric mechanical stresses generated during the deposition process on different layers generate constructive or destructive interference which results to spatially variable dynamic bulk modulus depending on the deposition orientations of layers.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Investigating and Optimizing the Lysate-Based Expression of Nonribosomal Peptide Synthetases Using a Reporter System

Lysate-based cell-free expression (CFE) systems are accessible platforms for expressing proteins that are difficult to synthesize in vivo, such as nonribosomal peptide synthetases (NRPSs). NRPSs are large (>100 kDa), modular enzyme complexes that synthesize bioactive peptide natural products. This synthetic process is analogous to transcription/translation (TX/TL) in lysates, resulting in potential resource competition between NRPS expression and NRPS activity in cell-free environments. Moreover, CFE conditions depend on the size and structure of the protein. Here, a reporter system for rapidly investigating and optimizing reaction environments for NRPS CFE is described. This strategy is demonstrated in E. coli lysate reactions using blue pigment synthetase A (BpsA), a model NRPS, carrying a C-terminal tetracysteine (TC) tag which forms a fluorescent complex with the biarsenical dye, FlAsH. A colorimetric assay was adapted for lysate reactions to detect the blue pigment product, indigoidine, of cell-free expressed BpsA-TC, confirming that the tagged enzyme is catalytically active. An optimized protocol for end point TC/FlAsH complex measurements in reactions enables quick comparisons of full-length BpsA-TC expressed under different reaction conditions, defining unique requirements for NRPS expression that are related to the protein’s catalytic activity and size. Importantly, these protein-dependent CFE conditions enable higher indigoidine titer and improve the expression of other monomodular NRPSs. Notably, these conditions differ from those used for the expression of superfolder GFP (sfGFP), a common reporter for optimizing lysate-based CFE systems, indicating the necessity for tailored reporters to optimize expression for specific enzyme classes. In conclusion, the reporter system is anticipated to advance lysate-based CFE systems for complex enzyme synthesis, enabling natural product discovery.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Perspectives on biorefineries in microbial production of fuels and chemicals

Microbes drive our complex biosphere by regulating the global ecosystem through cycling elements and energy. Humankind has barely begun leveraging this biotransformation capacity to impact global economies and ecologies. Advances in genetic engineering, molecular analysis, metabolic flux modeling, microbial consortia/biome mapping and engineering, cell-free bioproduction, artificial intelligence/machine learning and the ever expanding -omics frontiers have set the stage for paradigm changes to how humankind produces, uses, transforms, and recycles carbon and energy through microbes. Harnessing this enormous potential could drive a global bioeconomy and manage carbon at a planetary level but requires understanding and application at a grand scale across a broad range of science and engineering disciplines. The penultimate manifestation of these advances is the “bio-refinery”, which is often referenced, but is a long way from being fully developed as a global carbon management platform. Broadening the feed stocks, processing operations, and product portfolio to a sequential cascade optimizing the conversion as a whole instead of limited outputs could greatly advance deployment and stability of a bioeconomy.

09 BIOMASS FUELS↗

DOE OSTI2021

Carbohydrate-Containing Conjugated Polymers: Solvent-Resistant Materials for Greener Organic Electronics

Organic semiconducting polymers are exciting materials for electronic applications because of their good mechanical and optoelectronic properties. A major advantage of organic semiconductors is their solution processability. This allows access to a variety of simple and cost-effective device fabrication methods compared to the expensive, high-temperature processing methods required for silicon-based electronics. However, these materials often have low solubility, which limits their processing to toxic halogenated solvents. Also, their limited solubility often leads to interfacial mixing during device fabrication. Herein, this work explores the incorporation of environmentally friendly carbohydrate side chains in conjugated polymers to enhance processability in eco-friendly solvents. Moreover, a mild postprocessing treatment was designed to enable solvent resistance. Isoindigo-based polymers with varied ratios of acetyl-protected galactose side chains were synthesized to improve solubility in o-anisole in the protected state, while inducing solvent resistance through intramolecular hydrogen bonding in the deprotected state. Solvent resistance was confirmed both visually upon submersion in various solvents and using UV–visible spectroscopy. Importantly, the mild basic treatment to achieve solvent resistance has no negative impact on the electronic performance of these materials in organic field-effect transistors, even after subsequent submersion in various solvents, making them a valuable platform for the production of green processable multilayer electronics.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Microbial colonization and persistence in deep fractured shales is guided by metabolic exchanges and viral predation

Background: Microbial colonization of subsurface shales following hydraulic fracturing offers the opportunity to study coupled biotic and abiotic factors that impact microbial persistence in engineered deep subsurface ecosystems. Shale formations underly much of the continental USA and display geographically distinct gradients in temperature and salinity. Complementing studies performed in eastern USA shales that contain brine-like fluids, here we coupled metagenomic and metabolomic approaches to develop the first genome-level insights into ecosystem colonization and microbial community interactions in a lower-salinity, but high-temperature western USA shale formation. Results: We collected materials used during the hydraulic fracturing process (i.e., chemicals, drill muds) paired with temporal sampling of water produced from three different hydraulically fractured wells in the STACK (Sooner Trend Anadarko Basin, Canadian and Kingfisher) shale play in OK, USA. Relative to other shale formations, our metagenomic and metabolomic analyses revealed an expanded taxonomic and metabolic diversity of microorganisms that colonize and persist in fractured shales. Importantly, temporal sampling across all three hydraulic fracturing wells traced the degradation of complex polymers from the hydraulic fracturing process to the production and consumption of organic acids that support sulfate- and thiosulfate-reducing bacteria. Furthermore, we identified 5587 viral genomes and linked many of these to the dominant, colonizing microorganisms, demonstrating the key role that viral predation plays in community dynamics within this closed, engineered system. Lastly, top-side audit sampling of different source materials enabled genome-resolved source tracking, revealing the likely sources of many key colonizing and persisting taxa in these ecosystems. Conclusions: These findings highlight the importance of resource utilization and resistance to viral predation as key traits that enable specific microbial taxa to persist across fractured shale ecosystems. We also demonstrate the importance of materials used in the hydraulic fracturing process as both a source of persisting shale microorganisms and organic substrates that likely aid in sustaining the microbial community. Moreover, we showed that different physicochemical conditions (i.e., salinity, temperature) can influence the composition and functional potential of persisting microbial communities in shale ecosystems. Together, these results expand our knowledge of microbial life in deep subsurface shales and have important ramifications for management and treatment of microbial biomass in hydraulically fractured wells.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Post-inflationary dark matter bremsstrahlung

Dark matter may only interact with the visible sector efficiently at energy scales above the inflaton mass, such as the Planck scale or the grand unification scale. In such a scenario, the dark matter is mainly produced out of equilibrium during the period of reheating, often referred to as UV freeze-in. Here, we evaluate the abundance of the dark matter generated from bremsstrahlung off the inflaton decay products assuming no direct coupling between the inflaton and the dark matter. This process generally dominates the production of dark matter for low reheating temperatures where the production through the annihilations of particle in the thermal plasma becomes inefficient. We find that the bremsstrahlung process dominates for reheating temperatures T RH ≲ 10 10 GeV, and produces the requisite density of dark matter for a UV scale ≃ 10 16 GeV. As examples, we calculate numerically the yield of the dark matter bremsstrahlung through gravitation and dimension-6 vector portal effective interactions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2026

Techno-Economic Comparison of Molten-Salt Electrolysis and Carbothermic Reduction for the Production of Metallurgical-Grade Silicon

Metallurgical-grade silicon (MG-Si) is an important source material for many industrial applications, including the manufacture of alloys, solar photovoltaics, and electronics. The process to refine raw materials into MG-Si is energy-intensive, with the predominant method of submerged-arc furnaces requiring energy consumption of approximately 11–13 kWh/kg Si. Recent research has discussed promising methods for reducing the energy required for the silicon production process, including the use of molten-salt electrolysis (MSE), a technique that offers potential savings in energy consumption without requiring carbon inputs for the process. This paper presents a techno-economic study of a potential industrial-scale MSE plant for MG-Si production to evaluate the trade-offs between capital and operating costs of the system. Capital costs are sourced from recent MG-Si plants and an existing cost model developed for MSE processes that includes the size of the plant and the operating temperature among its inputs. The results show that MSE technology has the potential to be an economically cost-competitive option for MG-Si production if the technology successfully scales to industrial production and matures enough to allow for financing costs similar to that of a comparably sized submerged-arc furnace plant.

14 SOLAR ENERGY↗