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Results from the DOE Advanced Gas Reactor Fuel Development and Qualification Program

Modular HTGR designs were developed to provide natural safety, which prevents core damage under all design basis accidents and presently envisioned severe accidents. The principle that guides their design concepts is to passively maintain core temperatures below fission product release thresholds under all accident scenarios. This level of fuel performance and fission product retention reduces the radioactive source term by many orders of magnitude and allows potential elimination of the need for evacuation and sheltering beyond a small exclusion area. This level, however, is predicated on exceptionally high fuel fabrication quality and performance under normal operation and accident conditions. Germany produced and demonstrated high quality fuel for their pebble bed HTGRs in the 1980s, but no U.S. manufactured fuel had exhibited equivalent performance prior to the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program. The design goal of the modular HTGRs is to allow elimination of an exclusion zone and an emergency planning zone outside the plant boundary fence, typically interpreted as being about 400 meters from the reactor. To achieve this, the reactor design concepts require a level of fuel integrity that is better than that claimed for all prior US manufactured TRISO fuel, by a few orders of magnitude. The improved performance level is about a factor of three better than qualified for German TRISO fuel in the 1980’s. At the start of the AGR program, without a reactor design concept selected, the AGR fuel program selected to qualify fuel to an operating envelope that would bound both pebble bed and prismatic options. This resulted in needing a fuel form that could survive at peak fuel temperatures of 1250°C on a time-averaged basis and high burnups in the range of 150 to 200 GWd/MTHM (metric tons of heavy metal) or 16.4 to 21.8% fissions per initial metal atom (FIMA). Although Germany has demonstrated excellent performance of TRISO-coated UO2 particle fuel up to about 10% FIMA and 1150°C, UO2 fuel is known to have limitations because of CO formation and kernel migration at the high burnups, power densities, temperatures, and temperature gradients that may be encountered in the prismatic modular HTGRs. With uranium oxycarbide (UCO) fuel, the kernel composition is engineered to prevent CO formation and kernel migration, which are key threats to fuel integrity at higher burnups, temperatures, and temperature gradients. Furthermore, the recent poor fuel performance of UO2 TRISO fuel pebbles measured in Chinese irradiation testing in Russia and in German pebbles irradiated at 1250°C, and historic data on poorer fuel performance in safety testing of German pebbles that experienced burnups in excess of 10% FIMA [1] have each raised concern about the use of UO2 TRISO above 10% FIMA and 1150°C and the degree of margin available in the fuel system. This continues to be an active area of study internationally.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Low drift type N thermocouples in out-of-pile advanced gas reactor mock-up test: metallurgical analysis

Thermocouples are the most commonly used sensors for temperature measurement in nuclear reactors. They are crucial for the control of current nuclear reactors and for the development of GEN IV reactors. In nuclear applications thermocouples are strongly affected by intense neutron fluxes. As a result of the interaction with neutrons, the thermoelements of the thermocouples undergo transmutation, which produces a time dependent change in composition and, as a consequence, a time dependent drift of the thermocouple signal. Thermocouple drift can be very significant for in-pile temperature measurements and may render the temperature sensors unreliable after exposure to nuclear radiation for relatively short times compared to the life required for temperature sensors in nuclear applications. Previous experiences with type K thermocouples in nuclear reactors have shown that they are affected by neutron irradiation only to a limited extent. Similarly type N thermocouples are expected to be only slightly affected by neutron fluxes. Currently the use of Nickel based thermocouples is limited to temperatures lower than 1000 deg. C due to drift related to phenomena other than nuclear irradiation. As part of a collaboration between Idaho National Laboratory (INL) and the University of Cambridge a variety of Type N thermocouples have been exposed at INL in an Advanced Gas Reactor mock-up test at 1150 deg. C for 2000 h, 1200 deg. C for 2000 h, 125 deg. C for 200 h and 1300 deg. C for 200 h, and later analysed metallurgically at the University of Cambridge. The use of electron microscopy allows to identify the metallurgical changes occurring in the thermocouples during high temperature exposure and correlate the time dependent thermocouple drift with the microscopic changes experienced by the thermoelements of different thermocouple designs. In this paper conventional Inconel 600 sheathed type N thermocouples and a type N using a customized sheath developed at the University of Cambridge have been investigated. The rationale for the superior performance of the type N using a customized sheath developed at the University of Cambridge is explained in comparison with the behavior of conventional type N Inconel 600 sheathed thermocouples. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE Advanced Gas Reactor Fuel Development and Qualification Program Overview

AGR-3/4 post-irradiation examination and data analysis AGR-5/6/7 PIE and safety testing Supplemental fuel microanalysis and method development Fuel oxidation testing Air/moisture Ingress Experiment (AMIX) system development (deployed in FY23) Single particle testing in FITT Data management and analysis Fuel performance modeling

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A summary of the results from the DOE advanced gas reactor (AGR) fuel development and qualification program

Modular high temperature gas-cooled reactor (HTGR) designs were developed to provide natural safety, which prevents core damage under all licensing basis events. The principle that guides their design concepts is to passively maintain core temperatures below fission product release thresholds under all accident scenarios. The required level of fuel performance and fission product retention reduces the radioactive source term by many orders of magnitude relative to source terms for other reactor types and allows a graded approach to emergency planning and the potential elimination of the need for evacuation and sheltering beyond a small exclusion area. Achieving this level, however, is predicated on exceptionally high coated-particle fuel fabrication quality and excellent performance under normal operation and accident conditions. The design goal of modular HTGRs is to meet the Environmental Protection Agency (EPA) Protective Action Guides (PAGs) for offsite dose at the Exclusion Area Boundary (EAB). To achieve this, the reactor design concepts require a level of fuel integrity that is far better than that achieved for all prior U.S.-manufactured tristructural isotropic (TRISO) coated particle fuel.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Performance of Custom-Made Very High Temperature Thermocouples in the Advanced Gas Reactor Experiment AGR-5/6/7 During Irradiation [Slides]

Three thermocouple types were incorporated into the AGR-5/6/7 experiment: HTIR-TC, Cambridge Type N, and standard Type N. Prior to selecting these thermocouples, a development and testing program was conducted, and improvements made to the HTIR-TC design. Partly because of the extreme temperatures, the experiment has experienced a relatively high thermocouple failure rate. However, all capsules had at least three surviving thermocouples at the end of four cycles. In the high temperature regions, the HTIR-TCs suffered a lower failure rate compared to Cambridge Type N. One HTIR-TC operated at 1450–1500°C for 85 days without observable drift, which we believe to be the highest sustained temperature ever recorded in a reactor experiment. Three other HTIR-TCs operated at 1250–1400°C, also without observable drift.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Studying Unirradiated TRISO-coated Particles from the Second Advanced Gas Reactor Experiment

Combined precession electron diffraction and point resolved chemical imaging have been used to provide an analysis of the material structure and chemical information of unirradiated uranium oxy-carbide (14.0 wt% enriched) kernelled tristructural isotropic-coated (TRISO) coated particle fuel. The detailed microstructural analysis includes examination of the structure associated with kernel, IPyC and SiC layers, as well as the IPyC-SiC interface. The analysis serves as a baseline for future studies on the potential effects of fission product and defect release through intact SiC layers and possible grain restructuring with irradiation. The baseline microstructure is thereby identified to understand the subtle effects of fabrication that may influence fission product precipitate release associated with different fuel types. Results indicated a Si:C gradient in the SiC layer which could influence fission transport reactivity and the high resolution imaging at the IPyC-SiC interface shows the gradual chemical composition change at this interface.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Advanced Gas Reactor Fuel Specification Technical Bases

The technical bases for the TRISO-coated particle fuel specifications used by the AGR Program during its fabrication process development and fuel qualification efforts are provided based on historical HTGR fabrication experience in the U.S. and Germany and improvements and insights gained during execution of the AGR Program. The technical bases are provided for specified properties of the kernel, the TRISO coating layers, the fuel particle, and fuel compact in terms of fabricability considerations, in-pile fuel performance, and fission product release under normal and off-normal conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Drying Simulated Advanced Gas Reactor Fuel: Proving the Concept - 17637

Spent Nuclear Fuel (SNF) reprocessing is due to cease in the UK in 2018 and a new interim storage method may be required if it is found that pond storage is not viable beyond the 25 year period which is currently understood to be safe. Dry storage has been used elsewhere in the world for zircaloy and aluminium clad fuel and has been proposed for use in the UK, however since the UK's fuel is predominantly stainless steel (SS) clad, testing will need to be carried out to ensure that drying methods are suitable. This will require representative samples for macro scale drying tests. To date, little long term stored fuel has been examined. As a result, work has been carried out to try and ascertain whether the corrosion associated with long term storage leads to significant bound water and whether through wall cracks can be formed in intact lengths of SS tube. It was found that unlike an aluminium simulant, corroded SS showed no sign of water loss as a result of oxide dehydration during controlled drying by thermogravimetric analysis, and consequently bound water could be disregarded. It was also found that through wall cracks could be produced in an intact length of SS tube which would be suitable for macro scale drying tests. Some initial macro scale drying tests have been carried out using an alternative test piece with preformed cracks, and three distinct drying regimes to complete dryness have been detected. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE Advanced Gas Reactor Fuel Development and Qualification Program Overview

DOE AGR fuel development and qualification program overview to include TRISO fuel development and program elements, AGR timeline, Irradiation test results, performance evaluation results, major accomplishments and milestones over 12 months, and university-led TRISO related research projects.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

AGR-1, AGR-2, AGR-3/4, and AGR-5/6/7 DimensionalChange Analysis

A series of fuel irradiation experiments have been planned in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) to support the licensing and operation of the Advanced Reactor Technologies high temperature gas-cooled reactor. The advanced gas reactor (AGR) experiments are comprised of multiple independent capsules containing multiple cylindrical fuel compacts, placed inside of a graphite cylinder in ATR. The purpose of the AGR experiments is to provide data on fuel performance under irradiation, support fuel process development, qualify the fuel for normal operating conditions, provide irradiated fuel for accident testing, and support the development of fuel performance and fission product transport models. The advanced graphite creep (AGC) experiments provide irradiation creep data for design and licensing. To date, six irradiation campaigns have been completed: AGR-1 (December, 2006 – November, 2009); AGR-2 (June, 2010 – October, 2013); AGR-3/4 (December, 2011 – April, 2014); AGC-1 (September, 2009 – January, 2011); AGC-2 (April, 2011 – May, 2012); and AGC-3 (November, 2012 – April, 2014).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

UZrCN Synthesis via Arc Melting - A Novel Synthesis Study

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO2) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

36 MATERIALS SCIENCE↗

UZrCN Synthesis via Arc Melting

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO 2 ) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO 2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

UZrCN Formation via Arc Melting – A Novel Synthesis Study

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO2) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

36 MATERIALS SCIENCE↗