High-Temperature Irradiation-Resistant Thermocouple (HTIR-TC) Qualification Work
HTIR-TC Qualification work newsletter article for the FY22 ASI Spring Newsletter.
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HTIR-TC Qualification work newsletter article for the FY22 ASI Spring Newsletter.
Over the preceding ten years, continual research and development has been performed on the high temperature irradiation resistant thermocouple (HTIR-TC) by the team at Idaho National Laboratories (INL) High Temperature Test Laboratory (HTTL). The HTIR-TC has the capability of achieving high temperatures up to 1600°C or more. Further, the HTIR-TC has gone through many longevity tests both in and out of pile to show the amount of drift is minimal compared standard thermocouples. Key considerations for properties and materials of the HTIR-TC have been final diameter, ductility after heat treatment, and minimizing transmutation of materials during operation. Further, heat treatment and calibration processes have been established in order to consistently produce repeatable and reliable temperature readings. The current work provides further background for the standardization process of the HTIR-TC.
This report documents thermocouple testing performed in IRC Lab C-15 over a period of seven years. This testing supported selection and characterization of the thermocouple set used in the AGR-5/6/7 experiment. The following summary was taken directly from the report. Temperature measurement is a challenging aspect of very high temperature irradiation experiments because commonly used high-temperature commercial thermocouples such as platinum-rhodium (Types S, R, and B) and tungsten-rhenium (Type C), suffer dramatic drift because of neutron-induced transmutation. As a result, these types of thermocouples, which are used routinely for industrial temperature measurements outside of reactors, are used only in very special circumstances for reactor experiments. Conversely, because of their low neutron cross-sections, Type N thermocouples are affected to only a limited extent by neutron irradiation. However, the use of these nickel-based thermocouples is limited when the temperature exceeds 1050°C due to drift arising from minor alloying elements migrating from the thermocouple's metal sheath to the thermoelements. This change in the composition of the thermo-elements results in significant decalibration of the signal. The issues described above were recognized during the early planning stages of the final AGR experiment (designated AGR-5/6/7), and a thermocouple furnace testing program was performed over a seven-year period (2014-2019, 2021) to first select and then characterize the best thermocouple set for the high temperature regions of the AGR-5/6/7 irradiation experiment. The calculated temperature range of the AGR-5/6/7 experiment was 600–1500°C. For temperatures below 1000°C standard Type N thermocouples were deemed adequate. The furnace testing campaign identified two thermocouple types suitable for measuring temperatures above 1000°C, a Mo/Nb thermocouple developed at INL called HTIR-TC, and a Type N thermocouple developed by Cambridge University (called herein Cambridge Type N), which featured a custom high nickel alloy sheath. One of the original goals of the furnace testing program was to identify a thermocouple capable of low drift operation near the peak temperature expected in AGR-5/6/7, i.e., about 1400°C. The HTIR-TC design appeared promising in this regard, however a manufacturing difficulty proved to be a barrier and instead the furnace testing focused on drift performance at 1250°C. The manufacturing difficulty was that the Nb sheaths of the HTIR-TCs experienced extreme embrittlement when heat treated at 1600°C or greater. Heat treatment is needed to stabilize the emf output of this TC type, and the higher the heat treatment temperature the higher the peak temperature of stable operation. Because of the sheath embrittlement the heat treatment temperature had to be lowered to 1450°C resulting in a stable operating temperature of about 1250°C. One of the successes of the furnace testing program was identification of a shortcoming in the heat treatment procedure that had been traditionally used in the production of HTIR-TCs. The shortcoming was that the entire heated length of the HTIR-TC sensor was not being heat treated, but rather only the part of the sensor expected to experience temperatures above 1000°C. The problem manifested itself when the thermocouples were removed from the heat treat furnace and placed in another furnace with a different geometry, their indicated temperatures would be widely scattered, but mostly in the negative direction. The solution was to heat treat the entire heated length of the sensor. Since the deepest immersion depth in the AGR-5/6/7 experiment was about 40 inches, a heat treatment length of 48 inches was used. After this change was implemented, thermocouples which were moved into a new environment with a different temperature profile (i.e., a different furnace), produced accurate temperature measurements. Although assembly of the AGR-5/6/7 experiment was completed in September of 2017 (and irradiation begun in 2018), furnace testing of thermocouples continued in 2018 and 2019. The main purpose of this testing was to establish very long-term drift characteristics of the HTIR and Cambridge Type N thermocouples installed in the experiment. Representative thermocouples from the same lots as those installed in the AGR-5/6/7 experiment were used. Additionally, thermocouples of different designs, (particularly variations on the HTIR-TC design) were "piggy-backed" on this testing program to provide insights for instrumenting future very high temperature irradiation experiments. This two-year testing program demonstrated that HTIR-TCs and Cambridge Type N TCs could operate at 1250°C for up to 10,000 hrs (and in some cases longer) while experiencing negative drifts on the order of 2-4°C/1000 hrs. This performance was considered acceptable given the extreme operating environment the sensors faced.
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.
This article presents an instability model for the high-temperature irradiation-resistant thermocouple (HTIR-TC). Here the term instability defines the superposition of both drift and inhomogeneity of TC thermoelements occurring simultaneously. The HTIR-TC is an advanced thermocouple (TC) that uses the refractory metals niobium and molybdenum as sensing thermoelements for generating electromotive force (EMF) in a field of neutrons and at temperatures upward of 1,600°C. In the Advanced Gas Reactor (AGR) 5/6/7 tests conducted at Idaho National Laboratory’s Advanced Test Reactor (ATR), the HTIR-TCs showed low to moderate instability throughout the life of the test. The instability model reveals that HTIR-TCs can, when the operating temperature of the reactor fuel is normal, maintain performance throughout an 18-month refueling cycle typical of nuclear power plants, reflecting an instability of less than ±1%. The HTIR-TC is also qualified for incorporation into a test fixture during the testing of new fuels.
The High Temperature Irradiation Resistant Thermocouple (HTIR-TC) is the world’s leading temperature sensor for reactor fuel experiments and material test reactors (MTR), in general (e.g. Advanced Test Reactor, Massachusetts Institute of Technology Nuclear Reactor, etc.). Recently commercialized, the HTIR-TC provides real-time centerline and fuel cladding temperature measurements of reactor fuel experiments during irradiations. This provides direct information about fuel temperatures during Gen IV reactor, small modular reactor (SMR), and microreactor vetting processes. Further, the HTIR-TC recently won the 2019 R&D100 award under category: Analytical/Test.
This is a qualification report for the high-temperature irradiation-resistant thermocouple (HTIR-TC) developed by Nuclear Energy Enabling Technologies Advanced Sensors and Instrumentation program. Utilizing the Advanced Gas Reactor (AGR) 5/6/7 test conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory, the HTIR-TCs measured temperatures upwards of 1500°C during accident conditions. The HTIR TCs are thus qualified to perform and withstand an 18-month refueling cycle typical of nuclear power plants at the normal operating temperature, with a drift of less than ±1%. The HTIR-TC is also qualified for incorporating into a test fixture during new fuels tests.
The Advance Sensors and Instrumentation fiscal year report on the direct application of the HTIR-TC drift model on other commercial thermocouples. The Type N and K thermocouples are useful in irradiation environments up to 1100°C (or 1290°C for short bursts and/or single use), but over temperature and high fluence can cause the TCs to drift. The HTIR-TC drift model predicts the end use environment of temperature and irradiation and the total time scale to show the amount of drift a thermocouple will undergo. The model predicts that HTIR-TCs at full temperature range and fluence of 10^21 N/cm^2 will exhibit a drift of under -1%. The type N and K TCs will see a drift of -0.5% at the same fluence, but temperatures below 1100°C. Above this temperature the Type N and K TCs quickly de-calibrate and will give erroneous temperatures measurements.
The High Temperature Irradiation Resistant thermocouple (HTIR-TCs) has proven to be the nuclear temperature sensor. It outlast and outperforms all other commercially available thermocouples above 1100 °C inside reactor pressure vessels; also, recent calibration methods have pushed the HTIR-TC to accurately read temperatures through thermal transients during reactor shutdowns and restarts. The new temperature range of HTIR-TCs is from 0 °C to 1650 °C. The main objective of this study is to address manufacturing a more robust TC for handling and inserting into reactor experiments; to also apply the TC to a wider application. The TC has shown to be mainly susceptible to oxygen levels inside the heat treatment and calibration process and it is recommended that O2 levels be brought to as low as possible. However, through modeling efforts the O2 has been found to intercalate only within the first few layers of niobium on the outer sheath. Lastly, multiple materials were used for the sheath and insulators; all with similar outcomes when testing occurred over a long period of time.
The function and operation requirements for the high-temperature irradiation-resistant thermocouple (HTIR-TC) are set forth. A mission and product are proposed. The function and operational requirements involve temperature range, accuracy, drift, life, mechanical ruggedness, and response time. Each have a criterion set to establish a thermocouple that can withstand a typical 18-month nuclear power plant refueling cycle.
An established calibration procedure is presented for the high-temperature irradiation-resistant thermocouple (HTIR-TC). Standard calibration curves for both an individual (i.e. case by case basis) and common calibrations is shown. The error limits within ±3 σ are ±1% for the individual calibrations and ±2% for the common calibration.
The Advanced Gas Reactor -5/6/7 (AGR-5/6/7) experiment was the fourth and final experiment in the AGR experiment series and completed irradiation in July 2020. It serves as the formal fuel qualification test for the TRISO fuels under development by the US Department of Energy. This experiment was designed to irradiate fuel particles at temperatures ranging from 800°C ? 1500°C. The high end of the range created unique challenges for thermocouple-based temperature measurements. Commercially available high-temperature platinum-rhodium thermocouples (Types S, R, and B) and tungsten-rhenium thermocouples (Type C) suffer rapid decalibration due to transmutation of the thermoelements from neutron absorption. A special low neutron cross-section thermocouple system based on molybdenum/niobium thermoelements called High Temperature Irradiation Resistant thermocouple (HTIR-TC) has been under development at INL since circa 2004. Several examples of this thermocouple type were incorporated into regions of the test operating above 1200°C. For regions in the test operating in the 1000°C ? 1200°C range, high-performance versions of Type N thermocouples recently developed at Cambridge University were installed. Standard Type N thermocouples were used in regions of the test operating below 1000°C. A total of 54 thermocouples were incorporated into the test. A report of the performance of this large heterogenous set of thermocouples over the first third of the irradiation was previously provided (ANIMMA 2019). This follow-on paper discusses results from the balance of the experiment (Feb 2019 - July 2020). Special attention is focused on potential drift of thermocouples operating in the higher temperature regions.
This is a conference presentation ppt file. The following abstract is for the entire conference paper - which will later be the subject of a PRS artifact The Advanced Gas Reactor -5/6/7 (AGR-5/6/7) experiment was the fourth and final experiment in the AGR experiment series and completed irradiation in July 2020. It serves as the formal fuel qualification test for the TRISO fuels under development by the US Department of Energy. This experiment was designed to irradiate fuel particles at temperatures ranging from 800°C ? 1500°C. The high end of the range created unique challenges for thermocouple-based temperature measurements. Commercially available high-temperature platinum-rhodium thermocouples (Types S, R, and B) and tungsten-rhenium thermocouples (Type C) suffer rapid decalibration due to transmutation of the thermoelements from neutron absorption. A special low neutron cross-section thermocouple system based on molybdenum/niobium thermoelements called High Temperature Irradiation Resistant thermocouple (HTIR-TC) has been under development at INL since circa 2004. Several examples of this thermocouple type were incorporated into regions of the test operating above 1200°C. For regions in the test operating in the 1000°C ? 1200°C range, high-performance versions of Type N thermocouples recently developed at Cambridge University were installed. Standard Type N thermocouples were used in regions of the test operating below 1000°C. A total of 54 thermocouples were incorporated into the test. A report of the performance of this large heterogenous set of thermocouples over the first third of the irradiation was previously provided (ANIMMA 2019). This follow-on paper discusses results from the balance of the experiment (Feb 2019 - July 2020). Special attention is focused on potential drift of thermocouples operating in the higher temperature regions.
Development of in-core instrumentation is driven by the pursuit of safer, more economic energy production from the perspective of both existing nuclear reactors and Generation IV reactor designs. Idaho National Laboratory has developed high-temperature irradiation-resistant thermocouples (HTIR-TCs) for temperature sensing inside Generation IV nuclear reactors. These thermocouples are composed of phosphorus-doped niobium (Nb-P) and lanthana-doped molybdenum (Mo-LaO) thermoelements, an alumina (Al2O3) insulation, and a niobium sheath. HTIR-TCs require an initial heat treatment exceeding the maximum service temperature to stabilize the generated electromotive force (EMF) signal. The mechanism behind the stabilization of the HTIR-TCs through traditional heat treatment methods is understood; however, the traditional heat treatment method is expensive, time consuming, and results in a heterogeneous microstructure. Therefore, we investigated a rapid method for stabilization and microstructure homogeneity, through Joule heating. This work evaluates the impact of Joule heating on the thermoelements’ microstructures, chemical stability, and mechanical properties so as to determine the mechanisms by which stabilization of the EMF signal occurs. Accordingly, during the Joule heat treatment, a secondary Nb3P phase coarsened along the length of the Nb-P thermoelement, along with the formation of an interaction region at the Al2O3/niobium interface. The interaction between the alumina insulation and the Nb-P thermoelement was also observed within the Mo-LaO thermoelement. Joule heating induced stability within the generated HTIR-TC EMF signal via the formation of secondary phases within the Nb-P and the interaction between the alumina insulation and the thermoelements.
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