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Developing New Fuels for High Performance Research Reactors

The National Nuclear Security Administration (NNSA) Material Management and Minimization (M3) program works globally to minimize the civilian use of highly enriched uranium (HEU), a weapon-usable nuclear material. Supporting this effort, M3’s Office of Reactor Conversion and Uranium Supply is developing new fuels capable of converting research reactors from HEU fuel to high-assay low-enriched uranium (HALEU) fuel. Some of the remaining research and test reactors (RTRs) operating on HEU today have unique designs, fuel configurations, and demanding performance requirements that cannot be met with an existing regulatory-approved low-enriched uranium (LEU) fuel. M3, DOE’s national laboratories, and other industry partners are qualifying new high-density LEU fuels to convert these RTRs while maintaining their unique capabilities supporting a wide variety of science and technology research in areas such as medicine, industry, defense, education, and training. Current efforts are focused on two options for the remaining US high-performance research reactor conversions: a monolithic uranium 10wt% molybdenum (U-10Mo) fuel form and a dispersion uranium silicide fuel form. This paper reviews the history and status of M3’s fuel qualification efforts for the U-10Mo LEU fuel form.

Montgomery, Rose [ORNL] (ORCID:0000000286038936)↗

Natura Resources Molten Salt Research Reactor (MSRR) Fuel Workshop: Summary Report

Idaho National Laboratory (INL) hosted the Natura Resources team in Idaho Falls for a 3-day fuel workshop, July 16-18, 2024. The purpose of this workshop was to understand Natura’s fuel requirements, determine the feasibility of producing that fuel at INL, and define the scope of work that would enable fueled operation of the Natura MSR-1 being deployed at Abilene Christian University (ACU).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

(Oxy)hydroxides Formed on Aluminum Fuel Materials After Irradiation and Long-Term Wet Storage - 20354

The aluminum cladding of research-reactor fuel experiences general corrosion when in contact with water during in-reactor service and post-discharge wet storage, resulting in the formation of adherent aluminum (oxy)hydroxide films. These (oxy)hydroxides contain chemically-bound water that poses challenges for extended dry storage due to the risk of thermal or radiolytic decomposition releasing free water and/or hydrogen and oxygen gases. This study describes characterization of the (oxy)hydroxides present on several aluminum materials used in reactor operation and subsequently stored wet in the L-Basin storage facility at the Savannah River Site (SRS) for an extended period. Characterization data providing insight into the loading, composition, and morphology of (oxy)hydroxides to be expected on service-exposed aluminum cladding provides valuable benchmarks for designing adequate drying and dry-storage approaches. This work is part of a broader investigation to address knowledge gaps and technical data needs for dry storage of aluminum-clad spent nuclear fuel (ASNF), which included in-lab growth of (oxy)hydroxide films on aluminum alloy substrates to investigate formation behavior, investigation of drying methods to remove existing (oxy)hydroxides from ASNF cladding, and measurement of radiolytic yield of hydrogen from (oxy)hydroxide powders and films. In this study, (oxy)hydroxide films were characterized for three aluminum-alloy materials used in reactors and subsequently stored wet for up to approximately 40 years in L-Basin at SRS: one cropping from a Missouri University Research Reactor (MURR) fuel element (Al-6061 alloy), one cropping from a Universal Sleeve Housing (USH) (Al-6063 alloy), and one Mark-16B fuel assembly (either Al-6061 or Al- 6063). The USH and Mark-16B were used in SRS production reactors. Characterization of the as-received (oxy)hydroxides included scanning electron microscopy (SEM) in both plan-view and cross-section to characterize the (oxy)hydroxide layer's morphology, thickness, and structure. X-ray diffraction (XRD) was used to identify the chemical composition and distinguish between the various aluminum (oxy)hydroxides known to form under reactor and storage conditions. XRD analysis revealed both bayerite (Al(OH)3) and boehmite (AlOOH) on the surface of the MURR and USH samples, as well as bayerite, boehmite, and gibbsite (another Al(OH)3 polymorph) on the surface of the Mark-16B sample. The aluminum trihydroxides, bayerite and gibbsite, are typically associated with corrosion in low-temperature (<80 deg. C) water, while boehmite is expected to form at higher water temperature (>80 deg. C). The presence of bayerite on the USH, which is believed to have operated close to 90 deg. C, suggests that boehmite formed during in-reactor exposure was not protective against further hydroxide growth in low-temperature wet storage. Cross-section scanning electron microscopy (SEM) showed total (oxy)hydroxide layer thicknesses of ∼5- 10 μm for the MURR and ∼5-15 μm for the Mark-16B. The thickness of the USH's (oxy)hydroxide layer was indiscernible by the current mounting and imaging method, despite plan-view SEM and XRD confirming the presence of an (oxy)hydroxide layer. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Thermal Dehydration of Aluminum (Oxy)hydroxides on Fuel Cladding Material - 20200

The aluminum cladding of research-reactor fuel undergoes general corrosion with resulting formation of adherent aluminum (oxy)hydroxide films during in-reactor and post-discharge exposure to water under various conditions and temperatures. These (oxy)hydroxides contain chemically-bound water that poses challenges for extended dry storage due to the risk of thermal or radiolytic decomposition releasing free water and/or hydrogen and oxygen gases. This study comprised laboratory experiments of thermal drying behavior of aluminum (oxy)hydroxides to identify approaches for reducing bound water on fuel cladding prior to sealed dry storage. Effective drying strategies for adherent (oxy)hydroxides on fuel cladding will improve the safety of dry storage by mitigating potential avenues for additional corrosion and/or generation of flammable gases inside the storage canister. This work is part of a broader investigation to address knowledge gaps and technical data needs for dry storage of aluminum-clad spent nuclear fuel (ASNF), which included investigation of (oxy)hydroxide formation on aluminum alloy substrates immersed in water, characterization of service-grown films from ASNF, and radiolytic yield of hydrogen from (oxy)hydroxide powders and films. The current work comprises experimental thermal dehydration of aluminum trihydroxides (bayerite and gibbsite) characteristic of low-temperature (<80 deg. C) corrosion in water and aluminum oxyhydroxide (boehmite) characteristic of high temperature (>80 deg. C) corrosion in water. First, commercially produced (oxy)hydroxide powders (boehmite and gibbsite) were tested via thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). The effort aimed to identify or confirm key temperature ranges/thresholds for the thermal decomposition reactions, as well as impacts of ramp rate and hold times, for drying of isolated, high-surface-area (oxy)hydroxides. The information gleaned from powder tests was used to guide subsequent drying tests on adherent (oxy)hydroxide films grown on aluminum alloy substrates. TGA was used to analyze small samples of the aluminum coupons with adherent (oxy)hydroxide films. Specimens were characterized both pre- and post-drying using X-ray diffraction (XRD) to determine the film composition and scanning electron microscopy (SEM) to determine its morphology. Drying of adherent (oxy)hydroxide films was anticipated to pose additional complications relative to drying of (oxy)hydroxide powders. Anticipated challenges include achieving sufficient drying of the (oxy)hydroxide at low-enough temperature to avoid melting or other undesirable phase changes in the aluminum substrate and overcoming transport limitations of water through the thickness of a dense film or through a tortuous pore structure to reach the outer surface of the film. Inn addition, dehydration of (oxy)hydroxides significantly changes the film density, which may lead to substantial alterations in the morphology, including potential cracking and spalling of the film. TGA/DSC tests of gibbsite powders resulted in successful conversion to boehmite or alumina, depending on the maximum temperature reached. At low ramp rates (≤5 deg. C/min), the conversion to boehmite occurred around 300 deg. C (210-340 deg. C). XRD confirmed that boehmite was the only phase detected after tests reaching 450 deg. C. The transition to alumina occurred around 510 deg. C (470-550 deg. C), with XRD detecting only alumina after tests reaching at least 600 deg. C. Boehmite powders dehydrated to alumina at about 400 deg. C (330-460 deg. C) for coarse (77-μm particle diameter) powder and about 490 deg. C (420-520 deg. C) for fine (0.7-μm particle diameter) powder. For all powders tested, the maximum percent mass loss after drying to high temperature slightly exceeded the theoretical mass loss for complete dehydration of the stoichiometric (oxy)hydroxide to alumina, which is likely attributable to physisorbed water in the powder. Drying of a thick (∼8.6 μm), predominantly bayerite adherent film displayed a dramatic change in film morphology, with the initially continuous trihydroxide film cracking into sections on the order of 50 μm square and partially delaminating. The outermost layer of the film completely faked of in some regions. The layer exposed under the spalled oxide also displayed prominent cracking, with spacing on the order of 10 μm, but this surface layer appeared to remain completely adhered to the aluminum substrate. TGA showed mass losses per unit surface area up to ∼1.0 mg/cm{sup 2}. XRD characterization of the remaining oxide was inconclusive, with no crystalline phases detected. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analysis of H-Canyon Process Tanks in Preparation of Consolidation and Blending for HALEU Fuels

High-Assay Low- Enriched Uranium (HALEU) fuels are being developed to support the replacement of Highly Enriched Uranium (HEU) fuels used in U.S. High-Performance Research Reactors (USHPRR) as well as advanced nuclear power reactor designs. The projected demand for HALEU far exceeds the supply and studies are underway to assess various options to partially mitigate the potential short supply. The H Canyon facility at the Savannah River Site (SRS) Low Enriched Uranium (LEU) containing 4.95% U-235 from the reprocessing of highly enriched foreign and domestic research reactor fuel for the Tennessee Valley Authority’s (TVA) commercial power reactor market for several decades. The production of LEU at the H-Canyon facility can be readily transitioned to produce 19.75% HALEU solutions from the current separated inventory of purified HEU solutions in H-Canyon storage.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Proposed Subcritical Assembly for Nuclear Criticality Safety Training at the Oak Ridge National Laboratory

The design of a new subcritical assembly at Oak Ridge National Laboratory (ORNL) has been finalized. This design takes the feasibility study of the subcritical assembly performed in August 2020 to an implementable design. This subcritical assembly will support the Nuclear Criticality Safety Program (NCSP) training and education program. The addition of this subcritical assembly into the NCSP training and education will enhance the program by providing backup capacity for training if nuclear facility operations are disrupted at Sandia National Laboratories or the National Criticality Experiments Research Center; providing a new location that is more accessible to students in the Eastern portion of the United States; providing flexibility to support students from a diverse background (e.g., university students, foreign nationals). The proposed subcritical assembly uses legacy AGN-201M research reactor fuel plates that are available at the Y-12 National Security Complex. The final design of this subcritical assembly contains approximately 617 grams of 235 U as UO 2 powder distributed homogeneously in polyethylene. The fuel plates will have a graphite neutron reflector to obtain a core multiplication, M, from 10 to 20, corresponding to a $k_{eff}$ of 0.90 to 0.95, respectively. The subcritical assembly will be able to support at least four experiments for the training courses: (1) the addition of fissile material to the core (mass), (2) a core separation experiment (interaction), (3) the addition of moderators to the core (moderation), and (4) the addition of neutron absorbers to the core (poison/absorption). The subcritical assembly will be designed to be inherently safe—subcritical under all normal and abnormal conditions— and will provide the capability to conduct hands-on training to support NCSP and general nuclear criticality safety staff training and qualification goals.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

University of Missouri Research Reactor (MURR) LEU Fuel Fluid-Structure Interaction Analysis

The University of Missouri Research Reactor (MURR ® ) is one of five U.S. high performance research reactors (USHPRR), plus one critical facility, that are actively collaborating with the National Nuclear Security Administration (NNSA) Material Management and Minimization (M 3 ) Reactor Conversion Program to convert from highly enriched uranium (HEU, ≥ 20 wt.% U-235) to low-enriched uranium (LEU, < 20 wt.% U-235) fuel. A new type of LEU fuel with very high density, based on an alloy of uranium and 10 weight percent molybdenum (U-10Mo), is expected to allow the conversion to LEU of USHPRR that have been found unable to be converted with previously qualified uranium silicide-aluminum (U 3 Si 2 -Al) dispersion fuel. MURR has been working with the USHPRR Reactor Conversion (RC) Pillar at Argonne National Laboratory to perform fuel element design and fuel cycle performance analyses, steady-state thermal hydraulics safety analyses, and accident safety analyses in preparation for the conversion of MURR and to support a preliminary Safety Analysis Report (SAR) for conversion to LEU fuel. In this work, Fluid-structure interaction (FSI) analysis at the fuel element level, as compared to the fuel plate level of the previous work. is performed which models all components of the MURR LEU fuel element, including fuel plates and the supporting structures e.g., side plates, end fittings, and combs. Therefore, the effect of supporting structures on the coolant flow distribution, the fuel plate deflection, and the resulting coolant channel gap reduction can be evaluated. In addition to the nominal element geometry and flow rate, the tolerances in the geometry dimensions of coolant channel and plate thickness, the effect of a comb on plate deflection, and the uncertainty of the flow rate per element are considered in this work. The effect of comb on plate displacement is quantified through two bounding cases: the case assuming a perfect bond between the comb and plates and the case neglecting the comb effect. Note that in this analysis, the FSI has been decoupled from the other structural effects caused by irradiation (e.g., swelling and irradiation creep). Assessment of combined effects is planned for a later stage of this project.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DEVELOPMENT OF AN APPROACH FOR DOWNBLENDING AND DISPOSITION OF IRRADIATED GRAPHITE FUEL

The IGR reactor, a pulse-type test experimental reactor, reached full power in 1961. The reactor contains a center axial experimental ampoule that is subjected to a large pulse of neutrons (neutron flux maximum density of 7×1016 n/cm2·s, peak power 10GW) when the reactor is operated. The fuel form for the IGR reactor is graphite cubes and rods impregnated with highly enriched (90%) uranyl-dinitrate (UO2(NO3)2·6H2O). This fuel is eligible for return to Russia for reprocessing under the Russian Research Reactor Fuel Return program. However due to some technical and licensing issues it was decided to immobilize this fuel in Kazakhstan. The disposition approach thus selected for the spent HEU fuel involves down-blending of the fuel followed by cementation. Development of the process for down-blending and subsequent cementation requires a process that satisfies many criteria, including fissile content, compressive strength, permeability, and containment of radioactivity, among others. One key goal of the final product is to meet the criteria for termination of safeguards. This paper will describe the overall challenge associated with disposition of irradiated HEU graphite spent fuel, the identification of the objectives of the disposition process, and the constraints associated with development of the process and the waste form.

Gaines, Kris↗

IER 517: Molybdenum Critical Experiment Design [Slides]

In nuclear fuels, U-Mo metallic fuels are used in new space reactor designs and new research reactor fuels. MITR, MURR, and NBSR reactors plan on converting from different HEU fuels to a U-Mo HALEU fuel. In spend nuclear fuel, 95 Mo is one of the 15 main absorbing fission products in irradiated LWR fuel. This makes it important for criticality safety studies in transportation and reprocessing. In structural materials. Molybdenum is found commonly in alloys that make up the structural materials of nuclear reactors such as type 316 SS. Molybdenum helps to improve high temperature performance and corrosion resistance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Catalytic Effects of Silver in Iodine Reactors for Dissolved Used Nuclear Fuel

The dissolution of used nuclear fuel generates a variety of off-gasses including flammable hydrogen and other species that are a concern for environmental release. The H-Canyon facility at the Savannah River Site is currently dissolving aluminum-clad research reactor fuel from material test reactors and the High Flux Isotope Reactor (HFIR) using a mercury-catalyzed nitric acid flowsheet. Savannah River National Laboratory recently developed and deployed a Raman spectrometer to monitor the off-gas stream from the dissolution process. Results from these measurements indicated a lack of the expected hydrogen, nitrous oxide, and nitric oxide in the off-gas stream. It was proposed that the silver on the silver nitrate–coated berl saddles present in the reactors for iodine capture were acting as a catalytic hydrogen recombiner. Nitric oxide is readily oxidized to nitrogen dioxide under normal conditions, but it was unclear what happened to the nitrous oxide. A laboratory-scale iodine reactor was assembled and filled with silver nitrate–coated berl saddles to help ascertain the fate of nitrous oxide and hydrogen. Testing with this laboratory-scale reactor observed the recombination of hydrogen when a simulated dissolver off-gas was passed through the reactor containing silver nitrate–coated berl saddles at the approximate temperatures seen in H-Canyon. However, the nitrous oxide concentration was unchanged, suggesting a more complex process occurring within the off-gas stream before it reaches the iodine reactors at H-Canyon.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Panel Session 145: Challenges and Opportunities in Establishing a System for Transportation of SNF/UNF

Issues associated with establishing a SNF Transportation System in the U.S. are complex. In part, this is because in the US when discussing SNF, there are two distinct categories. The two categories represent significant differences in ownership, transportation-regulator, and even the physical characteristics of the SNF. Specifically, the physical differences in the SNF include size of the rods, associated quantities to be shipped, cladding material, and radionuclide content/enrichment. The first is commercial SNF (i.e., that associated with nuclear power plants), owned by utilities, until a permanent repository is built with DOE obligated by law to then assume the responsibility for shipping and ownership of the SNF. Since no-permanent repository currently exists, most commercial SNF is stored near the reactor in which it was installed, hence requiring no shipments. Although current shipments of commercial SNF are very limited, the few that do occur are generally performed to support a utilities SNF consolidation effort utility and for post irradiation examination/testing. However, with approximately 83,000 metric tons currently being stored at more than 70 sites around the U.S., when a permanent repository becomes available, the required number of shipments will be extensive. The second category is DOE and research reactor fuel. These fuel rods are generally much smaller in length than commercial fuel rods, with the quantity of rods transported in a shipment significantly less than the number of rods in a typical commercial fuel assembly. Currently, most of the SNF shipments within the U.S come from this category. DOE is currently managing about 2500 metric tons of heavy metal of SNF. This panel focused on updates and status of transportation of SNF/UNF. Panelists provided updates and information on continuing impacts, risk assessment, equipment (rail cars, handling, securement), possible rail routing, and proposed inspection equipment/routing prior to shipments. Panelists with presentations: Preparing for Nuclear Waste Transportation (Daniel Ogg); Challenges and Opportunities in Establishing a System for Transportation of SNF/UNF (Kathy Langan); UNF Transportation: Challenges and Opportunities (Michael Valenzano)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Neutron Source Facility of the National Science Center “Kharkiv Institute of Physics and Technology” at Kharkiv, Ukraine

Argonne National Laboratory developed, designed, and supported the construction of a state-of-the-art Neutron Source Facility (NSF) at the Kharkov Institute of Physics and Technology (KIPT) in Kharkov Ukraine, under the U.S. DOE NNSA Russian Research Reactor Fuel Return (RRRFR) program. Ukraine approved the return of all highly enriched uranium in the country to Russia prior to the 2012 Nuclear Security Summit in return for the RRRFR program to fund the development, the design, and the construction of the NSF. The facility is designed to produce medical isotopes, train nuclear professionals, support the Ukrainian nuclear industry, and provide experimental capabilities for performing reactor physics, materials, and basic science research. The NSF was successfully started and operated in August 2021. The NSF is the first facility of this type in the world, and it will be used to understand the physics of driven systems for energy production and the disposal of spent nuclear fuels. The NSF consists of a subcritical assembly using low enriched uranium (LEU) fuel driven with an electron accelerator. The NSF target design utilizes tungsten or natural uranium for producing neutrons through photonuclear reactions using 100-MeV electrons. The accelerator power is 100 KW, which produces 3x10 14 neutrons per second from the uranium target. The subcritical assembly is designed to obtain the highest possible neutron flux intensity with an effective neutron multiplication factor of less than 0.98. Passive safety, reliability, and environmental considerations were included in the NSF design. The NSF utilization study shows that this neutron source has the capability of producing different medical isotopes. Several horizontal neutron channels are incorporated for performing applied and basic research. The NSF is configured to accommodate future design upgrades and new missions. The facility design was approved by the Ukraine Academy of Sciences before starting the NSF construction. The construction, the equipment installation, and the operation of the different systems of the NSF were completed and approved by the Ukrainian regulators. In July 2020, the State Nuclear Regulatory Inspectorate of Ukraine (SNRIU) issued a license for the physical startup of the NSF. The construction of facility was completed in early 2021.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Evaluation of flow-induced plate deflection for University of Missouri research reactor low-enriched uranium fuel element

The University of Missouri Research Reactor (MURR), located on the campus of the University of Missouri in Columbia, Missouri, is one of the six United States (U.S.) High Performance Research Reactors (USHPRR), including one critical facility, that are actively collaborating with the U.S. Department of Energy (DOE) National Nuclear Security Administration (NNSA) Office of Material Management and Minimization (M3) Reactor Conversion Program to convert from highly enriched uranium (HEU, ≥20 wt% U-235) fuel to low-enriched uranium (LEU, <20 wt% U-235) fuel. A new type of very high-density LEU fuel based on a monolithic alloy of uranium and 10 wt% molybdenum (U-10Mo) is expected to allow conversion of some USHPRR, including MURR. In the design of its fuel elements, MURR is using thin parallel curved fuel plates separated by coolant channels. In this work, fluid-structure interaction (FSI) analysis of the MURR LEU fuel element is performed at the element level (as compared to the plate level analysis), which models all components of the LEU fuel element, including fuel plates and the supporting structures. Therefore, the effect of supporting structures on the flow distribution within the element and the fuel plate deflection are evaluated. In addition to the element nominal flow rate and dimensions, the tolerances in the geometry of the coolant channel and plate thickness, the effect of a comb on plate deflection, and the uncertainty of the flow rate per element are evaluated. For the LEU fuel plates, which are thinner than the current HEU plates, the predicted plate deflection is found to be small compared to the fabrication and assembly tolerances. Thus, the FSI-induced deflections are not expected to noticeably reduce the coolant flow rate or predicted safety margins in the limiting channels for the MURR LEU fuel element. In addition to the simulation work, a hydraulic performance test of the MURR LEU fuel element is currently being planned to support conversion to the use of LEU fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Feasibility Study for a Subcritical Assembly at the Oak Ridge National Laboratory

A conceptual design has been completed for a new subcritical assembly at Oak Ridge National Laboratory (ORNL). This subcritical assembly will support the Nuclear Criticality Safety Program (NCSP) training and education program to augment current subcritical assembly capabilities at Sandia National Laboratories (SNL) and at the National Criticality Experiments Research Center (NCERC). The proposed subcritical assembly uses legacy AGN-201M research reactor fuel plates that are available at the Y-12 National Security Complex. This subcritical assembly contains approximately 620 grams of 235 U as UO 2 particulates distributed homogeneously in radiation-stabilized polyethylene. The fuel plates will have a graphite neutron reflector to obtain a core multiplication, $M$, from 10 to 50, corresponding to a k eff of 0.9 to 0.95, respectively. The subcritical assembly will be able to support at least four experiments for the training courses: the addition of fissile material to increase neutron multiplication (mass), a core separation experiment (interaction), the effect of adding moderators to the core (moderation), and the effect of adding neutron absorbers to the core (poison/absorption). The proposed ORNL subcritical assembly will provide additional student bandwidth to support NCSP training courses and to provide for some backup capacity in the event that nuclear facility operations are disrupted at SNL or NCERC due to some unforeseen issue. The subcritical assembly will be designed to be an inherently safe subcritical assembly—subcritical under all normal and abnormal conditions—and it will provide the capability to conduct hands-on training to support NCSP and general nuclear criticality safety (NCS) staff training and qualification goals.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Zirconium Sludge Criticality Calculations in Large Process Tanks

The Savannah River Site’s H-Canyon facility has been tasked with accelerating the disposition of used research reactor fuels. • Future missions will involve dissolution of “Non-Aluminum” clad fuels – not easily dissolved – Nitric acid is not capable of dissolving stainless steel, Zirconium, and Hastelloy, clad fuels by itself • The electrolytic dissolver has been (re) selected as a disposition path for these fuels. 2

Devine, Nathan P.↗