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At least 1,063 records · Page 59
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

MSR Proliferation Resistance and Physical Protection White Paper

This document represents the status of Proliferation Resistance and Physical Protection (PR&PP) characteristics for the Molten Salt Reactor designs selected by the Generation IV International Forum (GIF) Molten Salt Reactor (MSR) provisional System Steering Committee (pSSC) as representatives of three broad classes of MSRs. The three classes of MSRs are: (1) Liquid-fueled with integrated salt processing, (2) Liquid-fueled without integrated salt processing, (3) Solid-fueled with salt coolant. The intent is to generate preliminary information about the PR&PP merits of the MSR Reactor Technology and to provide insights for optimizing their PR&PP performance for the benefit of MSR system designers. It updates the MSR analysis published in the 2011 report “Proliferation Resistance and Physical Protection of the Six Generation IV Nuclear Energy Systems”, prepared Jointly by the Proliferation Resistance and Physical Protection Working Group (PRPPWG) and the System Steering Committees of the Generation IV International Forum, taking into account the evolution of both the systems and the GIF R&D activities since its publication. The document, prepared jointly by the GIF PRPPWG and the GIF MSR pSSC, follows the high-level paradigm of the GIF Proliferation Resistance and Physical Protection Evaluation Methodology to investigate the Proliferation Resistance and Physical Protection features of the GIF MSR representative designs. For PR, the document analyses and discusses the proliferation resistance aspects in terms of robustness against State-based threats associated with diversion of materials, misuse of facilities, breakout scenarios, and production in clandestine facilities. Similarly, for physical protection, the document discusses the robustness against theft of material and sabotage by non-State actors.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
NASA NTRS1992

SP-100 reactor with Brayton conversion for lunar surface applications

Examined here is the potential for integrating Brayton-cycle power conversion with the SP-100 reactor for lunar surface power system applications. Two designs were characterized and modeled. The first design integrates a 100-kWe SP-100 Brayton power system with a lunar lander. This system is intended to meet early lunar mission power needs while minimizing on-site installation requirements. Man-rated radiation protection is provided by an integral multilayer, cylindrical lithium hydride/tungsten (LiH/W) shield encircling the reactor vessel. Design emphasis is on ease of deployment, safety, and reliability, while utilizing relatively near-term technology. The second design combines Brayton conversion with the SP-100 reactor in a erectable 550-kWe powerplant concept intended to satisfy later-phase lunar base power requirements. This system capitalizes on experience gained from operating the initial 100-kWe module and incorporates some technology improvements. For this system, the reactor is emplaced in a lunar regolith excavation to provide man-rated shielding, and the Brayton engines and radiators are mounted on the lunar surface and extend radially from the central reactor. Design emphasis is on performance, safety, long life, and operational flexibility.

Mason, Lee S.↗
NASA NTRS1990

Refractory metal alloys and composites for space power systems

Results are presented on recent studies of refractory-metal-alloy and refractory-metal-composite technologies for space power systems, with emphasis on work performed at the Lewis Research Center in support of the Ground Engineering System (GES) for the SP-100 reactor. Special attention is given to the mechanical properties of alloys with compositions Nb-1Zr and Nb-0.1Zr-0.1C (the PWC-11 alloy) and to advanced fiber-reinforced composites. The results to date indicate that, for the GES at a power level of about 100 kWe, the PWC-11 has attractive creep properties that will extend the capabilities of the SP-100 reactor compared to a similar system fabricated from Nb-1Zr. On the other hand, tungsten-reinforced Nb-1Zr composites were found to provide a ten-fold and four-fold creep strength over Nb-1Zr and PWC-11, respectively, at 1400 to 1500 K.

Stephens, R.↗
NASA NTRS2020

Higher Power Design Concepts for NASA's Kilopower Reactor

The successful testing of the Kilopower reactor during the KRUSTY (Kilopower Reactor Using Stirling TechnologY) experiment significantly reduced the risk to fly fission power systems by demonstrating stable reactor operation through nominal and severe simulated mission scenarios. The experiment validated the neutronics, heat transfer, and power conversion systems needed for 1 kilowatt of electrical power production from the Kilopower reactor. The need for higher power reactors to support human exploration missions to the moon and Mars has become increasingly important due to the urgency to put boots on the moon by 2024 and have a sustainable presence in the following years. This desire has prompted NASA to continue the development of the Kilopower reactor to extend the power up to 10 kilowatts of electricity in support of a lunar base. These 10 kilowatt units are expected to be used as standalone units or be ganged together to create a modular power grid for propellent production, human habitats, and robotic exploration to name a few. The Kilopower reactor was originally designed to produce electrical power from 1 to 10 kilowatts using the same highly enriched uranium fuel, sodium heat pipes, and Stirling convertors at the proper scale. Consideration has also been given to the use of low enriched uranium fuel for these missions and will be studied along with the other aspects of the reactor. This paper will focus on the design concepts and trades associated with the scale up of the Kilopower power conversion system and heat transfer system to support human exploration of the moon and Mars.

Gibson, Marc↗
DOE OSTI2025

Technical Assessment of Off-Gas System Technologies for Potential Use in Molten Salt Reactors

Molten salt reactors (MSRs) are a class of Generation IV advanced reactor technologies aimed to enhance and improve the safety, fuel utilization and cost-effectiveness of nuclear power generation. MSR concepts are based on using a molten salt mixture as a primary nuclear reactor coolant, while the fuel can be either directly dissolved in the coolant (i.e., fluid-fueled) or can be in a separate solid form (i.e., salt-cooled solid-fueled). MSRs can be operated in either thermal or fast neutron spectra, as simple fissile convertors, or breeder reactors (e.g., utilizing both fissile and fertile fuels), as well as accelerator-driven sub-critical reactors or transuranic element burners. Operation of MSRs will necessitate management and treatment of the off-gas streams released to the headspace of the reactor where, in some designs, a cover gas can be circulated to remove certain fission products and maintain an inert atmosphere. An inert MSR cover gas swept over or sparged into the salt will confine radionuclides emerging from the free surface, including radioactive noble and non-noble gases, aerosols, and volatile species. The elements and compounds of these species will have a wide range of thermochemical and physical properties, some of which will decay to different products in the off-gas stream. Therefore, system components used to manage and treat MSR off-gas streams will need to be robust under dynamic reactor and chemistry conditions to support adequate reactor performance by managing the composition and species in the salt coolant and cover gas space. Off-gas system components would perform as a radionuclide boundary to the reactor vessel and a primary means for preventing radionuclide release; therefore, they are of high safety significance for MSR operations. This report reviews various technologies and materials for potential implementation in the design of an MSR off-gas system per a general conceptual framework. The reviewed technologies operate based on scrubbing, capture, delay, or separation of species in the off-gas stream. These include molten hydroxide scrubbers, solid sorbents, delay off-gas systems, particle traps, and cryogenic distillation. Since aspects of an off-gas system will be design-specific, the approach is to provide general discussions on attributes of these technologies and materials, including target off-gas stream species, operational parameters and conditions of importance to decontamination factors, implementation maturity, system component monitoring, potential off-normal conditions and considerations for waste products. The information aims to support the U.S. Nuclear Regulatory Commission in their safety evaluations for MSR designs.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2025

Operational Experience and Development of a Reliability Model for the ATR Demineralizer System (Slides)

The Advanced Test Reactor (ATR) is a light water reactor with aluminum clad driver fuel. Strict limits are implemented on pH, conductivity, and filterable solids to assure the performance of the driver fuel limit corrosion of the primary coolant system (PCS) pressure boundary components. A bypass demineralizer system is used to maintain PCS coolant within allowable bands for each of the aforementioned variables. Unlike many other reactors, the ATR does not have a filtration system. As such, failure of ion exchange resin in the bypass demineralizer can defeat the purpose of the system and result in high filterable solids in the PCS. Power operations with high filterable solids is prohibited by a technical safety requirement. This paper discusses recent failures of the ATR bypass demineralizer system. The testing and analysis done to deduce the cause of the failures is covered, as well as short term mitigative steps that were taken. To prevent the likelihood of future issues, historical data from the ATR and industry is used to develop a reliability model of the ATR bypass demineralizer system. Evidence of radiolytic decomposition of ion exchange resin was found in the cause investigation. As such, special attention is given to ion exchange resin failure due to high radiation environments. The reliability model is used to develop the ATR testing and maintenance program. Specifically, limits on resin service life are discussed.

21 - SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLAN↗
DOE OSTI2025

Property Measurements of LiF-NaF-KF Molten Salts Doped with Corrosion Products and Oxygen

Measurements of thermophysical properties of molten salts are needed for modeling and simulation activities that support the development of molten salt reactor (MSR) technologies. Properties of interest including transition temperatures, phase behavior, heat capacity, density, volumetric thermal expansion, surface tension, viscosity, thermal diffusivity, thermal conductivity, and vapor pressure are being performed at Argonne. Results of these property measurements are suitable for use in evaluating reactor performance during startup and the early operating life of the reactor. Ingressions of oxygen and moisture into the fuel salt are expected to occur at different times during the operating life of the reactor due to system leaks, maintenance, and refueling activities. The presence of these environmental contaminants induces corrosion of structural materials. The introduction of corrosion-derived species, oxygen and moisture is expected to affect the physical and chemical properties of the salt and operation of the reactor. Previous work performed at Argonne evaluated the effects of fission product dopants on the thermal properties of eutectic LiF-NaF-KF (FLiNaK). Properties of FLiNaK are commonly used to represent those of fluoride-bearing fuel salts. Metallic corrosion products such as chromium and nickel ions together with dissolved oxygen are expected to affect system redox differently than the accumulation of fission products. Work summarized in this report was performed to measure the effects of corrosion products and dissolved oxygen on the phase transitions, and specific heat capacity of FLiNaK. Thermophysical property measurements were made using four salts that were prepared by doping aliquots of a eutectic mixture of FLiNaK with surrogate corrosion products. Controlled additions of CrF 3 and NiF 2 were used as surrogates for corrosion product contamination anticipated during extended reactor operations in which fuel salt is in contact with steel reactor components. Controlled additions of UF 4 from two sources containing known amounts of UO 2 at different concentrations were used to represent oxygen contamination. The phase transitions and specific heat capacities of the four salts were measured by using differential scanning calorimetry. Measurements were made at temperatures spanning the range of 500−900 °C, which is the expected operating range of MSRs. Measured property values were compared to values measured previously with eutectic FLiNaK without dopants. Differences between property values measured for the doped and non-doped salts were compared with the uncertainties of the measurements to determine the significance of the effect of corrosion products and oxygen on salt properties.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Multi-Physics System-level Simulations of a Generic Pebble Bed High-Temperature Gas Cooled Reactor with Coupled SAM/Griffin Model

A SAM model for a 200 MWth generic pebble bed high-temperature gas-cooled reactor (PBHTGR) is presented in this work. As an extension to the modeling effort from FY-22 (Ooi et al. (2022)), an improved core channel approach is used to model the pebble bed of the reactor. The improvement greatly simplifies the model and reduces the run time of the model. Furthermore, the SAM model is coupled to the Griffin reactor physics model from Stewart et al. (2021) using the MOOSE MultiApp system where neutronics calculations are performed by the Griffin model and thermal hydraulics calculations by the SAM model. Favorable predictions are produced by the SAM/Griffin coupled model for steady-state normal operating condition. A load-following transient is also simulated with the coupled model where the neutronics and thermal hydraulics responses of the core are predicted correctly by the model. A protected Pressurized Loss of Forced Cooling (PLOFC) accident is simulated with the SAM model, in which the reactor power is determined using the decay heat curve, and therefore the Griffin model is not needed and thus decoupled. A simplified RCCS (Reactor Cavity Cooling System) loop is added to the model to remove decay heat from the core during the transient. Qualitatively, the prediction by the SAM model matches the expected behavior of a PB-HTGR during a PLOFC accident.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2025

SPC-3184 Rev 7 MARVEL Reactor Structures Build to Print Fabrication Specification

Idaho National Laboratory (INL) is developing a microreactor to produce electrical power utilizing a small nuclear core and under the Microreactor Application Research Validation and Evaluation (MARVEL) program. This procurement specification defines the requirements for fabrication of the MARVEL Primary Coolant System (PCS), Fuel and Core System (FCS), and Reactor Sub-Structure Assemblies, including the Upper Confinement Structure.

21 - SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLAN↗
NASA NTRS2010

The Bosch Process-Performance of a Developmental Reactor and Experimental Evaluation of Alternative Catalysts

Bosch-based reactors have been in development at NASA since the 1960's. Traditional operation involves the reduction of carbon dioxide with hydrogen over a steel wool catalyst to produce water and solid carbon. While the system is capable of completely closing the loop on oxygen and hydrogen for Atmosphere Revitalization, steel wool requires a reaction temperature of 650C or higher for optimum performance. The single pass efficiency of the reaction over steel wool has been shown to be less than 10% resulting in a high recycle stream. Finally, the formation of solid carbon on steel wool ultimately fouls the catalyst necessitating catalyst resupply. These factors result in high mass, volume and power demands for a Bosch system. Interplanetary transportation and surface exploration missions of the moon, Mars, and near-earth objects will require higher levels of loop closure than current technology cannot provide. A Bosch system can provide the level of loop closure necessary for these long-term missions if mass, volume, and power can be kept low. The keys to improving the Bosch system lie in reactor and catalyst development. In 2009, the National Aeronautics and Space Administration refurbished a circa 1980's developmental Bosch reactor and built a sub-scale Bosch Catalyst Test Stand for the purpose of reactor and catalyst development. This paper describes the baseline performance of two commercially available steel wool catalysts as compared to performance reported in the 1960's and 80's. Additionally, the results of sub-scale testing of alternative Bosch catalysts, including nickel- and cobalt-based catalysts, are discussed.

Abney, Morgan B.↗
DOE OSTI2021

Comparison of Irradiated TRISO Fuel Radioactivity from Multiple Advanced Reactor Designs

The SCALE code system was used to model, deplete, and compare several different TRISO-fueled reactor designs: a helium-cooled prismatic reactor, a helium-cooled pebble-bed reactor (PBR), and a Fluoride-Lithium-Beryllium (FLIBE) molten-salt-cooled PBR. The purpose of this comparison was to understand how differences in the reactor designs affect the radioactivity of the fuel after discharge and whether those differences are significant. First, the various reactor designs were build and depleted in the TRITON module for each design and fuel enrichment. Then, the TRITON outputs were used to create burn-up dependent reactor libraries. These libraries were then used by ORIGEN to determine the activities of discharged fuel for each reactor, which were compared to generic Westinghouse 17x17 fuel. Overall, the results showed that short term decays are dominated by reactors with higher operating powers, and the reactor type, initial fuel enrichment, and maximum burn-up are of only secondary importance. Although this analysis only focuses on activities in becquerels, these dependencies are consistent with the expected behavior of decay heat. However, analysis of long- term time periods post-irradiation shows that the reactor type and maximum burn-up have strong impacts on the activities; initial fuel enrichment has a secondary impact while operating power is inconsequential. These results would be useful for analyses, such as dose assessment and modeling in post- release scenarios; normal fuel handling operations; and spent fuel transport, storage and disposal. Of particular interest, the results in this report show that analyses that focus on spent nuclear fuel of advanced reactors need to consider each parameter carefully. Unsurprisingly, if the correct operating power is not used in short term analyses, the results will not be correct. Perhaps unexpectedly, however, if the correct reactor type is not used, then the long term results will also be incorrect, especially for areas such as permanent disposal. Even though this report focuses on the total activity of nuclear fuel, it provides initial results on the effects of various input parameters and also provides a framework to extend the work into other analyses of spent fuel from advanced reactors, especially those employing TRISO fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1990

Safety and environmental constraints on space applications of fusion energy

Some of the constraints are examined on fusion reactions, plasma confinement systems, and fusion reactors that are intended for such space related missions as manned or unmanned operations in near earth orbit, interplanetary missions, or requirements of the SDI program. Of the many constraints on space power and propulsion systems, those arising from safety and environmental considerations are emphasized since these considerations place severe constraints on some fusion systems and have not been adequately treated in previous studies.

Roth, J. Reece↗
DOE OSTI2023

Transient Modelling of HTGR Thermal Load Follow in Modelica

The ability of nuclear power plants to load follow electrical power demand is particularly important as we move to higher variable renewable (VRE) energy production on low carbon energy grids. High temperature gas reactors (HTGRs) are capable of load following by adjusting thermal output, but their high temperatures and thermal inertia significantly impact the power transients they are able to follow. To aid investigation into new integrated energy systems with advanced reactors, it is necessary to have an open-source transient model of a full HTGR primary and secondary. This paper introduces two new open-source models for a HTGR and corresponding balance of plant (BOP) written for the HYBRID library developed at Idaho National Laboratory. A transient thermal load follow test case was taken by the work from Brits et al. to benchmark our open-source model against transient operation results from other proprietary codes that exist. The control scheme for the two new models in combination is discussed and a comparison of the response in transient load follow between the two codes performed.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Nuclear reactor support and seismic restraint with core retention cooling features

A nuclear island includes a nuclear reactor, a lateral seismic restraint, and a reactor core retention cooling system. The lateral seismic restraint includes a vertically oriented pin attached to one of the bottom of the lower vessel head and the floor underneath the nuclear reactor, and a mating pin socket is attached to the other of the bottom of the lower vessel head and the floor. The reactor core retention cooling system includes one or more baffles, optionally thermally insulating material, disposed alongside the exterior surface of a lower portion of the reactor pressure vessel including at least the lower vessel head. A plenum is defined between the one or more baffles and the exterior surface of a lower portion of the reactor pressure vessel. The one or more baffles may define a lower plenum inlet surrounding the lateral seismic restraint.

Edwards, Tyler A.↗
NASA NTRS1994

Method of decontaminating a contaminated fluid by using photocatalytic particles

A system for decontaminating the contaminated fluid by using photocatalytic particles. The system includes a reactor tank for holding the contaminated fluid and the photocatalytic particles suspended in the contaminated fluid to form a slurry. Light irradiates the surface of the slurry, thereby activating the photocatalytic properties of the particles. The system also includes stirring blades for continuously agitating the irradiated fluid surface and for maintaining the particles in a suspended state within the fluid. The system also includes a cross flow filter for segregating the fluid (after decomposition) from the semiconductor powder. The cross flow filter is occasionally back flushed to remove any semiconductor powder that might have caked on the filter. The semiconductor powder may be recirculated back to the tank for reuse, or may be stored for future use. A series of such systems may be used to gradually decompose a chemical in the fluid. Preferably, the fluid is pretreated to remove certain metal ions which interfere with the photocatalytic process. Such pretreatment may be accomplished by dispersing semiconductor particles within the fluid, which adsorb ions or photodeposit the metal as the free metal or its insoluble oxide or hydroxide, and then removing the semiconductor particles together with the adsorbed metal ions/oxides/hydroxide/free metal from the fluid. A method of decontaminating a contaminated fluid is also disclosed.

Cooper, Gerald↗
DOE OSTI2023

Analysis and Thermal Property Investigations into Ternary Actinide Chloride Salt Systems Containing UCl3 and PuCl3

While regulators, the scientific community, and MSR developers still lack access to literature data on the thermal properties of clean fuel salts, even less information is available on the properties of fuel salts containing impurities. It is essential to understand, benchmark, and predict crucial data on the changes in thermal properties of fuel salt systems due to impurities arising from moisture, corrosion, and reactor operation (i.e., fission products). This research focuses on two actinide fuel salts (1) to investigate a worst-case scenario buildup of actinide fission product in a NaCl-UCl3 eutectic fuel salt and (2) to investigate NaCl-PuCl3 eutectic salt after 1000 hours of operation in a natural circulation flow loop flow to determine if corrosion or atmospheric (moisture/oxygen) products are present. For the first salt, a conservative assumption or worst-case scenario, for fission product buildup in a fuel salt was investigated by adding PuCl3 to eutectic 67 mol% NaCl – 33 mol% UCl3 salt resulting in a ternary salt having a composition of 61 mol% NaCl – 30 mol% UCl3 – 9mol% PuCl3. Addition of PuCl3 to eutectic NaCl-UCl3 resulted in a ternary salt that had a higher melting temperature than either the NaCl-PuCl3 or NaCl-UCl3 binary eutectic mixture. Addition of PuCl3 also resulted in an increase in density which was expected. The second salt was extracted from a micro loop. The composition of the fuel (primary) salt prior to flow loop operations was determined to be 64 mol% NaCl – 36 mol% PuCl3, however, the post-flow loop salt showed increased levels of MgCl2 and NaCl changing the salt composition to 10 mol% MgCl2 – 63mol% NaCl – 26mol% PuCl3) indicating the primary salt interacted with the rinse salt. Analysis of the post flow loop salt detected low concentrations of Al, Ni, Co, Nb, and Zr, most likely corrosion products from the flow loop material of construction. Contamination of the fuel salt (with the rinse salt NaCl-MgCl2) decreased the density by approximately 10% and reduced the onset of melting temperature by 50 °C, from 451 °C to approximately 400 °C. Results from the fission product simulated salt (61 mol% NaCl – 30 mol% UCl3 – 9mol% PuCl3) and the corrosion product salt (10 mol% MgCl2 – 63mol% NaCl – 26mol% PuCl3) will be included in two separate manuscripts for submission to peer-reviewed journals.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Design Study for Bio-Oil Production from Biomass Using a Dual Fluidized-Bed Reactor

To evaluate the re-design and reconfiguration of a dual-fluidized bed (DFB) gasification system into a recirculating pyrolysis reactor, Computation Fluid Dynamic (CFD) simulations of the system were conducted. The Barracuda Virtual Reactor® computational particle fluid dynamic code was used to perform simulations of the pyrolysis process. Modeling of the chemical reaction kinetics for both gas phase and solid particle phase were included. The recirculating pyrolysis reactor shown in Fig. 1a is based on a bubbling-bed biomass pyrolyzer and a riser combustor to convert the remaining char. The operational differences in the re-configuration of the DFB gasification system into a recirculating pyrolysis system for the production of bio-oil are (1) replacement of a low-surface area inert bed material with a high-surface-area bed material that has acidic properties to provide catalytic activity for the production of bio-oil with reduced oxygen content, (2) lower temperature and residence time for bio-oil production from pyrolysis, (3) replacement of the fluidization gas in the bubbling bed pyrolyzer from steam to nitrogen, and (4) the reduction of pyrolyzer freeboard volume. The bed material used for catalytic pyrolysis is Sasol 300 (300-micron dia., bulk density 0.94 kg/l, and surface area 130 m2/g) and is a theta-alumina with mild acidity. This is in comparison with previous standard bed material Carbo HSP (430-micron dia., bulk density 2.01 kg/l, and surface area 0.03 m2/g) used for gasification. For bio-oil production, pyrolysis in the bubbling bed requires temperatures in the range of 550 C in comparison with gasification temperatures near 850 C. To attain this lower temperature requires management of the energy mass balances, with control of the bed material recirculation rate between bubbling bed pyrolyzer and riser combustor, the introduction of a nitrogen purge in the pyrolyzer, and adjusting the pressure balance between the two vessels. To extract bio-oil from the pyrolysis reactor with a snorkel, two different freeboard configurations were evaluated. In Fig. 1 b the existing high freeboard configuration is shown and in Fig. 1 c the reduced freeboard design is presented. The introduction of a nitrogen purge for the high free board configuration provided the highest bio-oil production from the CFD simulations. To decrease the bed-material circulation rate, primary and secondary air on the combustor side were reduced, and the pressure on the combustor was slightly increased. A portion of the biomass and bio-oil was observed to be transported to the combustor, leading to a smaller pyrolysis yield. The control of the pyrolyzer temperature is performed by controlling the circulation rate. Good fluidization of the bubbling bed and cascade PID control are required to keep the temperature from oscillating due to large time delay experienced when changing primary and secondary air. (a) (b) (c) Figure 1. (a) Dual Fluidized Bed pyrolysis system configuration, (b) mole fraction of nonpolar biooil in high freeboard configuration, and (c) mole fraction of nonpolar bio-oil in low freeboard configuration with nitrogen purge introduced in both configurations.

BASIC BIOLOGICAL SCIENCES,BIOMASS FUELS↗
DOE OSTI2022

Direct synthesis of branched hydrocarbons from CO 2 over composite catalysts in a single reactor

The thermocatalytic hydrogenation of CO 2 to hydrocarbons using a composite catalyst system in a single reactor under mild reaction conditions was investigated, by combining methanol synthesis, methanol dehydration and dimethyl ether homologation catalysts. High selectivity to isoparaffins, which are versatile precursors to sustainable aviation fuels, was achieved. The use of Cu/BEA significantly improved both the conversion of oxygenates and the hydrocarbon yield compared to HBEA by facilitating H-incorporation in the C-chain growth during the homologation reaction. A study of catalyst composition and reaction conditions revealed that nearly complete conversion of oxygenates was achieved using a stacked-bed configuration, providing high C-selectivity to C 4+ hydrocarbons (34.1% among all products and 95.5% in products excluding CO). The ability to completely convert oxygenates to hydrocarbons and achieve high CO-free selectivity to desired hydrocarbon products is unprecedented in CO 2 -to-hydrocarbon reports, and advantageous for downstream separation, as CO can be easily separated and recycled to improve overall hydrocarbon production in an integrated process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗