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DOE OSTI2024

FUEL PERFORMANCE SIMULATION OF HIGH BURNUP FUELS IN PLANNED INTEGRAL DESIGN BASIS ACCIDENT EXPERIMENTS

High burnup (HBu) fuel rods from the Byron Nuclear Generating Station (BNGS) were recently received at Idaho National Laboratory (INL) to support a variety of planned Nuclear Energy fuel cycle R&D objectives ranging from fuel performance, fuel recycle, and spent fuel research topics. Among these R&D activities, these fuel rods will be the subjects of multiple in-pile experiment programs at the Transient Reactor Test (TREAT) facility as well as detailed characterization and testing in the hot cells at INL and Oak Ridge National Laboratory (ORNL). TREAT RIA experiments are planned for the Nuclear Energy Agency Framework for Irradiation Experiments (FIDES) Joint Experimental Program called High burnup Experiments in Reactivity Initiated Accident (HERA) program. TREAT and ORNL-furnace LOCA experiments are part of the Department of Energy (DOE) Advanced Fuels Campaign (AFC) program U.S. consensus LOCA test plan, and the in-pile experiments have also been proposed in a FIDES project called Loss of Coolant-High Burnup (LOC-HBu). The results of these test programs will provide crucial data about safety performance enabling extended licensable burnup limits for these fuels. The purpose of this paper is to document fuel performance computational simulations of the BNGS fuel using the Bison code. The detailed assessments include (1) the irradiation history of the fuel to provide prediction of as-run fuel conditions and (2) extending the irradiated fuel conditions into the as-designed experiment conditions for the HERA-HBu RIA experiments and for the LOC-HBu LOCA experiments. The results of these assessments will inform post-irradiation examinations (PIE) of the BNGS parent rods and detailed final design of the planned experiments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Fuel Performance Simulation of High Burnup Fuels in Planned Integral Design Basis Accident Experiments

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Benchmark for Fuel Shuffling and Depletion for Pebble-Bed Reactors

Pebble bed reactors have specific operational characteristics when their fuel-cycle and fueling operations are considered. They are specifically distinguished by other type of nuclear reactor designs by their online fuel recycling scheme, where the fuel elements that have not yet reached discharge burnup can be reloaded and recycled continuously during normal operation. The fuel in a pebble bed reactor is not stationary and stochastically moves through the core once or several times during its lifetime, which allows them to operate without requiring a large excess reactivity hold for the burnup. However, this characteristic of pebble bed reactors introduces challenges in simulation, as each pebble can take many different trajectories through the core, its composition depends on the details of the irradiation history that is unique to its aggregated path through the core. For predicting the safety performance characteristics, such as source term, maximum fuel temperatures and fuel failure rates, etc., it is important to accurately incorporate the movement of pebbles through the core during their lifetime in a multi-physics simulation together with other phenomena. The equilibrium core analysis for pebble bed reactors are performed with multi-physics tools including fuel depletion in a multi pass reload coupled to the fuel movement. Currently, there are only a few legacy multi-physics simulation tools that can implement the pebble flow characteristics and perform equilibrium core analysis for pebble bed reactors. However, there are development efforts on-going under Department of Energy's Nuclear Energy Advanced Modelling and Simulation program and also in private industry for including these capabilities into their modelling and simulation tools. Any new development in the modelling and simulation tools needs to be validated by using tools such as experiments, analytical solutions or code-to-code benchmarks. In this work, a code-to-code benchmark for the equilibrium core analysis capability of pebble bed reactors was developed. Multiple cases were identified to capture different fuel cycle strategies that can be used in PBRs. The results of each case are presented in terms of overall equilibrium core characteristics: the discharge burnup; spatial burnup distribution; spatial isotopic distributions; axial and radial neutron flux distributions and power history of fuel elements per pass through the core for both a prototypical pebble bed High Temperature Gas-cooled Reactor and a prototypical pebble bed Fluoride-salt cooled High temperature Reactor.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Catalytic Reduction of Carbon Monoxide to Liquid Fuels with Recyclable Hydride Donors

Solar light absorption and catalysis are physically separated processes in natural photosynthesis. Natural cofactors, such as nicotinamide adenine dinucleotides (NADH), transport electrons and hydrogen to regulate and activate enzymes at remote locations. The physical separation of light absorption from catalysis provides some inspiration for artificial photosynthesis. One rather extreme implementation is to use copper wires to transport carriers from photovoltaic cells to dark electrodes, where catalysis occurs. Indeed, with a futuristic electrical grid powered solely by photovoltaics, solar capture could be separated from catalysis by hundreds of miles. An alternative approach, that bares more similarity to natural photosynthesis, employs mobile NADH/NAD + -like species that shuttle between the light absorber and a proximate, yet unilluminated, location where catalysis occurs. Additionally, such a remote approach to solar photocatalysis was recently proposed for the reduction of carbon oxides, CO 2 and CO, to methanol by cascade catalysis. This developing artificial photosynthetic approach offers the promise of catalytic generation of methanol and oxygen gas with sunlight as the sole energy source and CO 2 and water as the only chemical feedstocks. This Viewpoint evaluates the strengths and weaknesses of this approach with an emphasis on CO reduction catalysis with photorecyclable hydride donors while looking forward to what might reasonably be achieved with continued research.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2020

Analysis of a 100-W Regenerative Fuel Cell Demonstration

A 100-W regenerative fuel cell (RFC) demonstration was successfully completed at the NASA Glenn Research Center on December 11, 2014. This effort was funded by Advanced Space Power Systems milestone and represented the first demonstration of passive laboratory-scale stacks arranged as an RFC, consisting of a non-flow-through fuel cell and a static-feed electrolyzer. Once developed, these stacks present the potential to minimize system mass, volume, and parasitic power in comparison to existing terrestrial electrochemical systems and nonnuclear power generation options. Testing involved the fuel cell powering a simulated load then recycling fuel cell product water by subsequently electrolyzing it to regenerate hydrogen and oxygen gases for fuel cell operations. A total of five cycles were completed over a 2-week period, yielding cell voltage data for stack performance and quality measures for regenerated reactants. Overall, round-trip efficiency was calculated to be 47.4 percent. Gas crossover was observed in electrolyzer gas products, as residual gas analysis showed 1.1 percent hydrogen in oxygen and 0.4 percent oxygen in hydrogen. Fuel cell product water was determined to be more acidic and conductive and have a higher fluoride content when compared to deionized water.

fuel cell↗

DOE OSTI2026

Advanced Facility Design and AI/ML Enabled Safeguards to Establish Secure, Economical Recycling of Fast Reactor Fuels (Final Scientific/Technical Report)

The project, "Advanced Facility Design and AI/ML Enabled Safeguards to Establish Secure, Economical Recycling of Fast Reactor Fuels," represents a significant advancement in nuclear fuel recycling technology. It integrates cutting-edge multimodal sensor fusion, machine learning (ML), and digital twin (DT) technologies to address challenges in material safeguarding, process optimization, and regulatory compliance for pyroprocessing facilities. This research has significantly enhanced the understanding of pyrochemical fuel recycling processes by developing innovative tools and methodologies. The Multimodal Safeguards Monitoring Unit (MSMU) combines electroanalytical techniques, Raman spectroscopy, and differential thermal analysis (DTA) to enable high-fidelity, near-real-time material accountancy measurements. Machine learning techniques, such as Long Short-Term Memory (LSTM) autoencoders, are utilized to detect anomalies in material balances and sensor data, improving the reliability of safeguards monitoring. Additionally, digital twin technology has been established to provide real-time system-level monitoring and diagnostics, integrating physics-based models with sensor data to optimize process safety and efficiency.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

Identifying Challenges in Safeguards for Metallic Fuel Fabrication Facilities

As new advanced reactors gain popularity, there is an increasing interest in metallic fuel fabrication for fast reactors. While metallic fuels themselves are not a new idea, as many of the first reactors employed metallic fuels, new designs, compositions, and fabrication methods are appearing throughout the nuclear community. As the interest grows and facilities are constructed, both domestic and international safeguards will need to be heavily involved to support safeguards-by-design (SBD) measures from the start. This work compiles a review of historical and modern fuel types and fabrication methods, fabrication processes, safeguards gaps, and potential safeguards solutions. Metallic nuclear fuel types have been around for many decades and were included in some of the first reactors including the Experimental Breeder Reactor (EBR)-I and -II, the Fermi 1 reactor, the Integral Fast Reactor (IFR), and the Dounreay Fast Reactor (DFR). These reactors used various compositions including pure uranium (U) metal, U-zirconium (Zr) alloys, plutonium (Pu)-aluminum (Al) alloys, U-fissium (Fs) alloys, U-Pu-Zr alloys, and U-molybdenum (Mo) alloys [1, 2, 3, 4, 5]. These small alloying additions are included to improve the material properties of the pure U metal. The alpha-phase U (stable below 661C) suffers elongation in one direction causing grain boundary cracking and increasing creep rate due to irradiation growth, thermal cycling, and preferential crystal orientation. It is ideal to utilize the gamma-phase U (typically stable above 769C) by adding small amounts of alloying elements such as Zr or Mo to stabilize this phase down to room temperature [3]. Additionally, some research has been focused on U with transuranic (TRU) elements present, typically coming from the used fuel recycling process. Including these elements in fast reactor fuel can aid in the reduction of nuclear waste by burning minor long-lived actinides. However, the additions of TRU elements can cause concerns to arise when trying to fabrication or safeguard metallic fuels. A typical metallic fuel element is shown in Figure 1. Sodium is added into the cladding to create a thermal bond between the fuel slug and cladding wall. The fuel slug is then inserted and the end plug is welded on to the top of the fuel element. A gas plenum is left to create a headspace for gaseous fission products to escape rather than continue to build in the fuel itself [1, 5]. Other fuel element geometries exist as well, such as the Lightbridge twisted cruciform geometry shown in Figure 2 [6]. This design allows for better cooling performance and provides room for fuel rod swelling without impacting the fuel rod diameter. There are many different fabrication methods for metallic fuels, which is one of the many benefits of these fuel types. Many of these fabrication methods are relatively easy and cost-efficient. The most popular fabrication method is injection casting, sometimes called vacuum induction melting (VIM), shown in Figure 3 [4, 8, 9, 7, 10]. This method was largely used for EBR-II fuel fabrication. The injection casting system is contained inside of a vessel consisting of a Y2O3-coated graphite crucible surrounded by an induction coil with ZrO2-coated quartz molds suspended above the crucible. The fuel feedstock is placed inside of the graphite crucible and melted using the induction furnace. The induction furnace utilizes a dual frequency with the high frequency melting the feedstock and the low frequency causing stirring of the melted feedstock to form a homogeneous mixture. The mixture is heated to approximately 1600C in an argon environment. The vessel is evacuated and then the quartz molds are lowered into the graphite crucible containing the molten metal and the vessel is repressurized to inject the metal fuel upwards into the molds. The molds are removed and then shattered to release the fuel slugs. This fabrication method was used to fabricate 39,000 metallic fuel pins for EBR-II. While injection casting has been the most common metallic fuel fabrication method throughout the decades, many other methods have been explored including low-pressure gravity casting, microwave casting, continuous casting, centrifugal casting, coextrusion, and many others [11, 12, 8, 13, 14, 15]. Some of these methods aim to mitigate challenges that arise with americium (Am) volatilization during the casting process for TRU-containing fuel feedstocks, an issue with injection casting. Coextrusion is one of the methods explored at the Idaho National Laboratory (INL) and has been utilized for the initial fabrication tests of Lightbridge's unique fuels, as well as other metallic fuels with cladding coextruded. In this process, large billets are formed and machined and then inserted into a molten salt bath for approximately 30 minutes. The billets are then loaded into the extrusion press and extruded. This process can be seen in Figure 4 [15].

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Possible impacts of molten salt reactors on the International Monitoring System

Molten salt reactors (MSRs) are gaining support as many countries look for ways to increase power generation and replace aging nuclear energy production facilities. MSRs have inherently safe designs, are scalable in size, can burn transuranic wastes from traditional solid fuel nuclear reactors, can store excess heat in thermal reservoirs for water desalination, and can be used to produce medical isotopes as part of the real-time liquid-fuel recycling process. The ability to remove 135 Xe in real time from the fuel improves the power production in an MSR because 135 Xe is the most significant neutron-absorbing isotope generated by nuclear fission. Xenon-135, and other radioactive gases, are removed by sparging the fuel with an inert gas while the liquid fuel is recirculated from the reactor inner core through the heat exchangers. Without effective abatement technologies, large amounts of radioactive gas could be released during the sparging process. This work examines the potential impact of radioxenon releases on samplers used by the International Monitoring System (IMS) to detect nuclear explosions. Here, atmospheric transport simulations from seven hypothetical MSRs on different continents were used to evaluate the holdup time needed before release of radioxenon so IMS samplers would register few detections. Abatement technologies that retain radioxenon isotopes for at least 120 d before their release will be needed to mitigate the impacts from a molten salt breeder reactor used to replace a nuclear power plant. A holdup time of about 150 d is needed to reduce emissions to the average level of current nuclear power plants.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2022

Zero carbon solid-state rechargeable redox fuel for long duration and seasonal storage

Here, this work presents a unique thermochemical process for charging magnesium-manganese-oxide-based solid-state rechargeable redox fuel. High-temperature heating of the processing furnace can be driven by either renewable electricity or concentrated solar power. The simple recyclable fuel charging concept is based on a tubular falling bed reactor with countercurrent oxygen-depleted gas flow for complete heat recuperation. The main focus of this work is achieving solid flowability at high temperatures (1,450°C) and extracting chemically charged solid at ambient temperature with minimal energy loss. The operation strategies described in this work have enabled consistent magnesium-manganese-oxide particle flow up to 1,450°C. The measured extent of the thermal reduction reaction after cooling the particles is more than 90% of the fully reduced state at equilibrium. The thermal-to-chemical efficiency and overall system efficiency are 96% and 35% respectively, which are the highest reported for thermochemical fuels to date.

25 ENERGY STORAGE↗

DOE OSTI2025

Implementation of fuel management multi-cycle optimization capabilities in RAVEN optimization framework

Optimization in nuclear fuel-management assists the core reload engineer with finding optimal out-of-core and in-core strategies. RAVEN is INL’s open source software that is equipped with fuel-management optimization capabilities including single-cycle, single- and multi-objective optimization of pressurized water reactors (PWRs) loading patterns (LP) of a fresh core using genetic algorithm (GA) and non-dominated sorting genetic algorithm (NSGA-II). In practice, however, medium and long term planning of fuel-management needs a multi-cycle approach, where the history and availability of fuel assemblies is considered in the optimization process. In this paper, we present a description of an initial expansion of RAVEN fuel-management optimization capabilities for a multi-cycle optimization framework. N-th cycle optimization capabilities that account for the unique history of recycled fuel assembly in the core were added. The multi-cycle optimization approach taken is formulated as a cycle-wise optimization problem where out-of-core decisions are used to onset each cycle optimization. Out-of-core decisions are managed externally to the in-core optimization by a fuel inventory management module. A proof-of-concept optimization problem is also presented.

42 - ENGINEERING↗

DOE OSTI2025

Non–linear bonding trends in maleonitrile-1,2–dithiolate complexes of the transuranium actinides

The trivalent actinides are produced in the nuclear fuel cycle during power production and provide the largest long-term radiation dose in used nuclear fuel. It is ideal for these elements to be removed from used nuclear fuel for disposal and a necessity for fuel recycling. A key challenge to this is the similarity of chemical behavior of the trivalent actinides to the lanthanides that are also present as fission products in used fuel. Thus far, some of the most effective separations of actinides from lanthanides utilise chelating agents containing sulfur moieties such as dithiophosphinates that selectively bind to actinide ions because of a greater bond covalency relative to lanthanide ions. Typically, greater differences between actinide and lanthanide ions are observable the more ligands and chelators bonds have a covalent character. Here, a series of complexes of the trivalent actinides Np(III) through Cf(III) (excluding Bk(III)) with maleonitrile-1,2-dithiolate (mnt 2– ) are synthesized along with their lanthanide counterparts (La(III) – Nd(III), Sm(III) – Gd(III), Dy(III)), in order to characterize the nature of chemical bonds with these metal ions and a polarizable, non-innocent, sulfur-donor ligand. The metal-sulfur bonds in these complexes trend shorter than measured for lanthanides with equivalent ionic radii. However, particularly large deviations are observed in the neptunium and plutonium complexes in both structure and bonding, resulting in a nonlinear bond length trendline for the actinide series. Density Functional Theory (DFT) calculations with Quantum Theory of Atoms in Molecules (QTAIM) and Natural Bond Order (NBO) analyses indicate that for the neptunium and plutonium complexes, the presence of increased 5f-orbital participation, energy degeneracy of the metal and ligand orbitals, and the structure packing result in shortened M–S bonds. The stabilization of the energy of the 5f-orbitals and the decrease in f-contribution to bonding orbitals in the later actinides results in structural properties more similar to the lanthanide complexes.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2020

An Enhanced Safeguards Approach for Accelerator Driven Systems utilized to Close the Fuel Cycle

Further to our previous safeguards approach for Accelerator Driven Systems, which focused on estimates of fissile material production using relevant proton accelerator systems and corresponding safeguards needs for fuel storage, the subcritical reactor, and spent fuel storage material balances areas, this report is more expansive and considers utilization of ADS for either burning of transuranics or breeding of fissile materials. We find that the recycled fuels likely intended for ADS will be thermally and radioactively hot to such a degree that it is likely reprocessing and fuel fabrication will have to be co - located with the ADS reactor facility to avoid impractical hot fuel transportation issues. As such, we consider in detail the full ADS system to include material balance areas for spent fuel receiving, reprocessing, storage & cooling, fuel fabrication, subcritical reactor area, and waste storage & handling. Furthermore, aqueous - based separation methods like PUREX cannot tolerate the intense heat of the ADS fuels, so pyroprocessing will likely be required. With these considerations, we developed an Enhanced Safeguards Approach for ADS beyond the work done in our first report, and conclude that significant diagnostic development is needed , a nd provide safeguards recommendations. We have also included an appendix regarding some country programs, in particular the Chinese ADANES burner/breeder program a nd the Indian thorium - based breeder program.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1975

Environmental considerations

A comparison was made between the environmental impact of the present nuclear-heated process and the currently commercial hydrogen-producing process utilizing coal for heating, i.e., the Lurgi coal gasification process. This comparison is based on the assumption that both plants produce the same quantity of H2, i.e., 269 cu m/sec of approximately the same purity, that all pollution abatement equipment is of the same design and efficiency for both the Lurgi process and the nuclear process, and that the energy required for the fresh nuclear fuel and the fuel recycle is generated in a power plant which is also provided with pollution abatement equipment. The pollution caused by the auxiliary units is also taken into account. As regards process water usage, the data show that the water required for the nuclear route, including the nuclear fuel production, is approximately 78% of that required for the Lurgi route.

Source record↗

DOE OSTI2023

Cummins R-SOFC System Development

The overall purpose of this project was to reduce the Reversible-Solid Oxide Fuel Cell (R-SOFC) system cost by developing two technologies, an improved cell design and the incorporation of an ejector in the fuel recycle loop instead of a blower. A Simulink model of the baseline SOFC system was developed and calibrated with experimental test data. The R-SOFC system model was built by integrating GT Suite developed models of the steam generation components into the baseline Simulink SOFC system model. The ability to run the stack in SOEC operating mode was also added to the model. The system model was used to explore the ability of the R-SOFC system to meet operational constraints on Steam/Carbon ratio and H2 concentration on the fuel side electrode. A CFD ejector model was developed and used to explore a range of ejector design parameters, leading to the final ejector design that was prototyped for testing. A prototype steam ejector was first tested in a laboratory environment using room temperature air. The steam ejector was subsequently tested using the full hot recycle loop with all relevant heat exchangers and steam generation components. The test conditions utilized temperatures, pressures, and flow rates expected in an R-SOFC application. Throughout the experimental testing work, ejector performance test data was used to improve and then validate the CFD ejector model. A CFD cell model was developed and used to optimize thermal gradients, voltage, and cost of a new cell substrate design. A CFD comparison of co-flow and cross-flow cell designs informed the decision to use a co-flow design for the new cell substrate. Multiple rounds of CFD simulation were used to improve the cell design to minimize the variation in air and fuel distribution across cell channels and to minimize the variation in air and fuel distribution across different cells in the stack. A few prototypes of the new cell substrate design were produced and validated in a laboratory environment by thermally spraying and verifying that they met established manufacturing specifications. The cell manufacturing process was adjusted in order to bring these metrics within acceptable tolerances. Cummins’ internal calculations show that the new cell design reduces cost ~50% compared to the baseline cell, while the ejector + superheater/boiler concept reduces cost of the recycle loop by ~40%. The impact of these cost reductions on the cost of producing H2 will depend on the specific system where they are applied. Therefore, a Techno-Economic Analysis was completed using system cost as a variable, and showing how the NREL Current and Future system costs translate into H2 production cost.

Henrichsen, Lars↗

DOE OSTI2020

Dissipative Assembly of Macrocycles Comprising Multiple Transient Bonds

Abstract Dissipative assembly has great potential for the creation of new adaptive chemical systems. However, while molecular assembly at equilibrium is routinely used to prepare complex architectures from polyfunctional monomers, species formed out of equilibrium have, to this point, been structurally very simple. In most examples the fuel simply effects the formation of a single short‐lived covalent bond. Herein, we show that chemical fuels can assemble bifunctional components into macrocycles containing multiple transient bonds. Specifically, dicarboxylic acids give aqueous dianhydride macrocycles on treatment with a carbodiimide. The macrocycles are assembled efficiently as a consequence of both fuel‐dependent and fuel‐independent mechanisms; they undergo slower decomposition, building up as the fuel recycles the components, and are a favored product of the dynamic exchange of the anhydride bonds. These results create new possibilities for generating structurally sophisticated out‐of‐equilibrium species.

Hossain, Mohammad Mosharraf↗

DOE OSTI2020

Overcoming Oxidation State-Dependent Spectral Interferences: Online Monitoring of U(VI) Reduction to U(IV) via Raman and UV–vis Spectroscopy

Analytical characterization of chemical processes is an essential component of both industrial processes and fundamental studies. Applicable techniques abound, but optical spectroscopy has the unique combination of being easily incorporated into on-line (in-situ) monitoring probes and can also provide abundant chemical information (concentration, oxidation state, speciation). However, this abundance of chemical information can make applying optical spectroscopy to complex chemical processes challenging. This is particularly evident in the bulk electrolysis of U(VI) to U(IV), an essential preparatory step in some nuclear fuel recycling schemes. Starting and product materials have interfering spectral signatures in both electronic and vibrational spectroscopies, making accurate and real-time analysis difficult to achieve. In this paper, we discuss the application of optical spectroscopy to the on-line monitoring of a bulk electrolysis process and the methods utilized to analyze data as well as characterize the efficiency and mechanism of U(IV) generation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Spectroscopic Online Monitoring: Using a Multi-Track Visible Spectrometer to Facilitate a Mass Balance Study in a Simulated TALSPEAK Process

Nuclear energy is a promising low-carbon energy candidate to meet the increased demand for green energy, where the integration of fuel recycling can have significant benefits for material usage and waste reduction. Utilizing in situ monitoring tools can provide ample opportunities to better control and safeguard nuclear material recycle processes while also offering knowledge and insight into real-time solution properties. The simultaneous measurement of analytical targets in multiple process locations can enable real-time mass balance and material accountancy calculations. This is demonstrated here with a mass balance study of Nd 3+ on countercurrent aqueous/organic metal extraction within a single centrifugal contactor. The Nd 3+ concentration was simultaneously monitored at the inlets and outlets of both aqueous and organic phases using a visible absorbance detector that allowed for the simultaneous measurement of up to six locations. The Nd 3+ concentration was calculated by using chemical data science algorithms, where model training sets were collected on a single track of the detector. The discussion includes addressing the challenges of using a model collected on a single track and applying it as a model across the other tracks on the detector. Each track of the detector corresponds to one measurement location on the contactor. The difference in the integrated moles of Nd 3+ between the inlet and outlet at the end of the experiment was near zero, indicating that the mass balance of this experiment was maintained. Overall, the online spectroscopic monitoring was able to follow changing solution conditions and accurately measure the concentration of Nd 3+ in different locations within the contactor system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Sensor Fusion: Comprehensive Real-Time, On-Line Monitoring for Process Control via Visible, Near-Infrared, and Raman Spectroscopy

On-line monitoring based on optical spectroscopy provides unprecedented insight into the chemical composition of process streams or batches. Amplifying this approach through utilizing multiple forms of optical spectroscopy in sensor fusion can greatly expand the number and type of chemical species that can be identified and quantified. This is demonstrated herein, on the analysis of used nuclear fuel recycling streams: highly complex processes with multiple target and interfering analytes. The optical techniques of visible absorbance, near infrared absorbance, and Raman spectroscopy were combined to quantify plutonium (III, IV, VI), uranium (IV, VI), neptunium (IV, V, VI), and nitric acid. Chemometric modeling was used to quantify analytes in process streams in real-time and results were successfully used to enable immediate process control and generation of a product stream at a set composition ratio. This represents a significant step forward in the ability to monitor and control complex chemical processes occurring in harsh chemical environments.

47 OTHER INSTRUMENTATION↗