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Initial Comparison of Baseline Physical and Mechanical Properties for the VHTR Candidate Graphite Grades

High-purity graphite is the core structural material of choice in the Very High Temperature Reactor (VHTR) design, a graphite-moderated, helium-cooled configuration capable of producing thermal energy for power generation as well as process heat for industrial applications that require temperatures higher than the outlet temperatures of present nuclear reactors. The Baseline Graphite Characterization Program is establishing accurate as-manufactured mechanical and physical property distributions in nuclear-grade graphites by providing comprehensive data that captures the level of variation in measured values. In addition to providing a thorough comparison between these values in different graphite grades, the program is also carefully tracking individual specimen source, position, and orientation information in order to provide comparisons both in specific properties and in the associated variability between different lots, different billets, and different positions from within a single billet. This report is a preliminary comparison between each of the grades of graphite that are considered “candidate” grades from four major international graphite producers. These particular grades (NBG-18, NBG-17, PCEA, IG-110, and 2114) are the major focus of the evaluations presently underway on irradiated graphite properties through the series of Advanced Graphite Creep (AGC) experiments. NBG-18, a medium-grain pitch coke graphite from SGL from which billets are formed via vibration molding, was the favored structural material in the pebble-bed configuration. NBG-17 graphite from SGL is essentially NBG-18 with the grain size reduced by a factor of two. PCEA, petroleum coke graphite from GrafTech with a similar grain size to NBG-17, is formed via an extrusion process and was initially considered the favored grade for the prismatic layout. IG-110 and 2114, from Toyo Tanso and Mersen (formerly Carbone Lorraine), respectively, are fine-grain grades produced via an isomolding process. An analysis of the comparison between each of these grades will include not only the differences in fundamental and statistically-significant individual strength levels, but also the differences in the overall variability in properties within each of the grades that will ultimately provide the basis for predicting in-service performance. The comparative performance of the different types of nuclear-grade graphites will naturally continue to evolve as thousands more specimens are fully characterized with regard to strength, physical properties, and thermal performance from the numerous grades of graphite being evaluated.

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Comparison between the Strength Levels of Baseline Nuclear-Grade Graphite and Graphite Irradiated in AGC-2

This report details the initial comparison of mechanical strength properties between the cylindrical nuclear-grade graphite specimens irradiated in the second Advanced Graphite Creep (AGC-2) experiment with the established baseline, or unirradiated, mechanical properties compiled in the Baseline Graphite Characterization program. The overall comparative analysis will describe the development of an appropriate test protocol for irradiated specimens, the execution of the mechanical tests on the AGC-2 sample population, and will further discuss the data in terms of developing an accurate irradiated property distribution in the limited amount of irradiated data by leveraging the considerably larger property datasets being captured in the Baseline Graphite Characterization program. Integrating information on the inherent variability in nuclear-grade graphite with more complete datasets is one of the goals of the VHTR Graphite Materials program. Between “sister” specimens, or specimens with the same geometry machined from the same sub-block of graphite from which the irradiated AGC specimens were extracted, and the Baseline datasets, a comprehensive body of data will exist that can provide both a direct and indirect indication of the full irradiated property distributions that can be expected of irradiated nuclear-grade graphite while in service in a VHTR system. While the most critical data will remain the actual irradiated property measurements, expansion of this data into accurate distributions based on the inherent variability in graphite properties will be a crucial step in qualifying graphite for nuclear use as a structural material in a VHTR environment.

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HDG-1 Graphite Preirradiation Data Package Report

This report documents all pre-irradiation examination material-property measurement data for graphite specimens that are going to be used within the first high dose graphite (HDG) -1 irradiation capsule. The two new HDG capsules signify a major change to the AGC Experiment. HDG-1 and HDG-2 will replace the last two Advanced Graphite Creep (AGC) capsules (AGC-5 and AGC-6) which were designed to irradiate graphite at the extreme upper operational temperatures for a very-high-temperature reactor (VHTR) design, 1100°C. These very high temperature AGC-5 and AGC-6 capsules have been repurposed to re-irradiated specimens (from AGC-2, AGC-3, and AGC-4) at the lower temperatures of 600°C and 800°C. HDG-1 will be irradiated at 600°C and HDG-2 will be irradiated at 800°C. By re-irradiating the previous AGC specimens a total maximum neutron dose of around 15 dpa (displacements per atom) can be achieved for all major graphite grades at irradiation temperatures of 600°C and 800°C. Specimens in the HDG-1 capsule are made up of previously irradiated specimens from the AGC-2 capsule and unirradiated specimens prepared for the now discontinued AGC-5 capsule. Utilizing the irradiated specimens, a maximum neutron dose of around 15 dpa is anticipated. These new maximum dose levels will provide irradiated material property data over a total neutron dose range of 1-15 dpa at a temperature of 600°C when combined with the previous AGC-1 and AGC-2 irradiation data. This will provide quantitative data necessary for predicting the irradiation behavior and operating performance of new nuclear graphite grades for use within high temperature reactor designs. Similar to previous AGC test trains, HDG-1 includes the major graphite grades (IG-110, NBG-17, NBG-18, PCEA, and 2114) as well as adding the very fine-grain grade IG-430 which is of interest to the Molten Salt Reactor (MSR) designs. Also new to the HDG-1 capsule are 90 smaller geometry specimens designated as pencil specimens. These specimens take up only one third the space of a standard creep size specimen. This increased number of specimens will enhance property measurement statistics because they will provide 3 times the control specimen data at a position that would otherwise only have a single measurement.

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ECAR-3051 As-Run Physics Analysis For The AGC-3 Experiment Irradiated In The ATR

This Engineering Calculations Analysis Report (ECAR) documents the results of the Advanced Test Reactor (ATR) detailed physics analyses performed to calculate the displacements per atom (DPA) and the fast neutron fluence (E > 0.1 MeV) of the Advanced Graphite Creep (AGC) experiment, AGC-3, irradiated in the ATR East Flux Trap (EFT) (see Figure 1) during ATR Cycle 152B, Cycle 154B, Cycle 155A, and Cycle 155B. This ECAR also reports the neutron and photon heat rates for the materials of the AGC-3 experiment for ATR Cycle 152B. The results for these evaluations and analysis are reported herein.

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ECAR-2322 As-Run Thermal Analysis Of The AGC-2 Experiment

The second Advanced Graphite Creep (AGC-2) experiment was designed to irradiate various types of graphite specimens at a temperature of 600°C. The specimens were irradiated in an instrumented leadout capsule experiment in the south flux trap of the ATR during cycles 149A, 1498, 1508, 151A, and 1518. Temperature was monitored using twelve thermocouples located at various elevations in the reactor core, and a helium-argon gas mixture was used for gas gap temperature control of the specimens. The purpose of this analysis is to calculate specimen temperature using measured data on reactor power and helium-argon gas flows, and as-run calculations of heating rates and displacement per atom (DPA) in graphite. The accuracy of the model is assessed by comparing measured and calculated thermocouple temperatures. Uncertainty in gas gaps may preclude an accurate temperature calculation. In these cases, adjustments are made to the thermal model in order to reconcile the measured and calculated thermocouple temperature and to ensure the accuracy of the calculated specimen temperature.

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ECAR-3386 AS-RUN THERMAL ANALYSIS OF THE AGC-3 EXPERIMENT

The third Advanced Graphite Creep (AGC-3) experiment was designed to irradiate various types of graphite specimens at a temperature of 900°C. The specimens were irradiated in an instrumented leadout capsule experiment in the east flux trap of the ATR during cycles 152B, 154B, 155A, and 155B. Temperature was monitored using twelve thermocouples located at various elevations in the reactor core, and a helium-argon gas mixture was used for gas gap temperature control of the specimens. The purpose of this analysis is to calculate specimen temperature using measured data on reactor power and helium-argon gas flows, and as-run calculations of heating rates and displacement per atom (DPA) in graphite. The accuracy of the model is assessed by comparing measured and calculated thermocouple temperatures. Uncertainty in gas gaps may preclude an accurate temperature calculation. In these cases, adjustments are made to the thermal model in order to reconcile the measured and calculated thermocouple temperature and to ensure the accuracy of the calculated specimen temperature.

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ECAR-1406 AS-RUN NEUTRONIC ANALYSIS OF THE AGC-1 EXPERIMENT IRRADIATED IN THE ATR SOUTH FLUX TRAP

This Engineering Calculations Analysis Report (ECAR) documents the results of the Advanced Test Reactor (ATR) detailed physics analyses performed to calculate the displacements per atom (DPA) and the fast neutron fluence (E > 0.1 MeV) of the Advanced Graphite Creep (AGC) experiment, AGC-1, irradiated in the ATR South Flux Trap (SFT) (see Figure 1) during ATR Cycle 145A, Cycle 145B, Cycle 146A, Cycle 146B, Cycle 147A, Cycle 148A and Cycle 148B. The results for these evaluations and analysis are reported herein.

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ECAR-2291 AS-RUN PHYSICS ANALYSIS FOR THE AGC-2 EXPERIMENT IRRADIATED IN THE ATR

This Engineering Calculations Analysis Report (ECAR) documents the results of the Advanced Test Reactor (ATR) detailed physics analyses performed to calculate the displacements per atom (DPA) and the fast neutron fluence (E > 0.1 MeV) of the Advanced Graphite Creep (AGC) experiment, AGC-2, irradiated in the ATR South Flux Trap (SFT) (see Figure 1) during ATR Cycle 149A, Cycle 149B, Cycle 150B, Cycle 151A, and Cycle 151B. This ECAR also reports the neutron and photon heat rates for the materials of the AGC-2 experiment for ATR Cycle 149B. The results for these evaluations and analysis are reported herein.

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Comparison of Irradiated and Unirradiated Graphite Oxidation Performance

This work examines the oxidation behavior of NBG-25 graphite using irradiated specimens and (not irradiated) companion specimens from the Advanced Graphite Creep (AGC) Experiment. Irradiated and companion specimens were quartered, split into four small samples, to enable four oxidation test runs for each (0.5 inch diameter by 0.25 inch tall) piggyback button obtained from the AGC Experiment inventory. These split samples were oxidized in air in a thermogravimetric analyzer (TGA) and benchmarked against observations with separately sourced same-grade specimens of three geometries oxidized either in the TGA or in a vertical furnace built and operated to satisfy the specifications of ASTM D7542. The study considers both irradiation damage and relief of damage by thermal annealing. A range of isothermal oxidation temperatures were tested for specimens exposed to a similar irradiation environment, nominally 6.5 dpa at 650°C. To assess the dose dependency of observed oxidation behavior, specimens with a range of irradiation exposures (up to 6.8 dpa) were tested at the single oxidation temperature of 650°C. In the conventional analysis (rate determined over the 5-10% mass loss range) any annealing effects appear to be negligible, while irradiation to ~6.5 dpa may double or triple the subsequent oxidation rate. However, examination of rate with extent of reaction (over incremental ranges from initial onset up to 5% mass loss) illustrates that (at least for ~6.5 dpa) irradiation initially inhibits oxidation. Slower rates of oxidation than companion split samples are clearly indicated across all oxidation temperatures tested up to ~0.5% mass loss. Over the range of 0.5-1% mass loss, regardless of normalization strategy, there is no statistically meaningful difference in oxidation rate. However, beyond 0.5% mass loss oxidation of the irradiated sample becomes progressively faster than the companion sample (up to the 10% mass loss level observed).

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Summary of Graphite Data Stored within NDMAS

The Graphite Technology Development Project provides data to support the design of graphite core components within specific reactor service conditions of the next generation of high-temperature, gas-cooled nuclear reactors. Physical, mechanical, and thermal properties of nuclear grade graphite were characterized for specimens that were unirradiated, irradiated, and irradiated under various stress conditions. The material properties include diameter, length, mass, density, compressive strength, tensile strength, flexural strength, modulus, resistivity, thermal diffusivity, and thermal expansion coefficient. Baseline graphite specimens are unirradiated from different grades (2114, IG-110, NBG-17, NBG-18, and PCEA) and different types used in different characterization tests (compressive, flexural, tensile, one-inch cylinder, and quarter-inch cylinder). The Advanced Graphite Creep (AGC) irradiation specimens are from a much larger number of grades and cylinder types (creep, piggyback, and pencil). For baseline graphite, characterization data for 7,756 specimens extracted from thirteen graphite billets were captured to the NDMAS database. For AGC experiments, four irradiation campaigns have been completed: AGC-1, AGC-2, AGC-3, and AGC-4. The ongoing HDG-1 (High-Dose Graphite) experiment, which began irradiation with Cycle 168B on August 26, 2020, includes specimens previously irradiated in AGC-2 in addition to the specimens originally destined for AGC-5.. Besides the characterization data, the AGC data includes irradiation monitoring and physics data representing the irradiation conditions of AGC specimens. Currently, all data for AGC-1, AGC-2, and AGC-3 have been captured to the NDMAS database. Only AGC-4 pre-irradiation and irradiation monitoring data have been captured, and HDG-1 pre-irradiation data are in process of being captured for unirradiated specimens. To date, a total of 38,149 material property records have been captured into NDMAS database for baseline and AGC specimens. All characterization data are qualified for use according to their perspective data verification reports. For the AGC irradiation campaigns, a total of 41,502 qualified physics calculation records were added for AGC-1, AGC-2, and AGC-3. Finally, a total of 173,698,505 AGC irradiation monitoring data records (thermocouple temperature, gas flow rate, gas pressure, gas moisture, applied load, and specimen displacement) have been captured to NDMAS; the majority of those records (~94%) are qualified data records.

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AGC-4 As-Run Uncertainty Analysis

The concept of measuring neutron flux (or fluence rate) with activation foils has existed since the late 1940s and is a well-used methodology. Activation foils are selected for their unique isotopic cross sections that create reaction products with desirable properties: relatively simple radioactive decay scheme, measurable quantities of gamma-rays or betas, and half-lives appropriate for the irradiation and decay durations of the experiment. The activation materials, deemed flux wires, fluence wires, dosimeters, or flux foils, are fabricated to have a mass appropriate for the irradiation as well so the measurement using a radiation detector following the irradiation is sufficient but not overwhelming in terms of total activity. Activation measurement results are expressed in terms of reaction rate, which can then be used to “adjust” the neutron spectrum. The Advanced Graphite Creep (AGC)-4 experiment contained 26 flux wire packages, each containing an iron and a niobium wire inside a vanadium capsule. For all stackup positions, the value of fast to thermal neutrons is higher than expected, but the total neutron fluence is near the predicted value of ~2 x 1022 n/cm2. As compared to the predicted neutron spectrum, there are four takeaways in the results as compared to the predicted ATR irradiation: 1) Additional fast (fission) neutrons present, 2) Spectrum hardening due to temperature, 3) Spectrum hardening due to container attenuation, 4) Total neutron fluence is close to predicted values. Since the neutron energy spectrum is a key parameter when attributing neutron damage in materials, the adjusted energy-dependent spectrum and the total neutron fluence results from the dosimeters can be incorporated for future calculations.

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AGC 2 Irradiated Material Properties Analysis

The Advanced Reactor Technologies Graphite Research and Development Program is conducting an extensive graphite irradiation experiment to provide data for licensing of a high temperature reactor (HTR) design. In past applications, graphite has been used effectively as a structural and moderator material in both research and commercial high temperature gas cooled reactor designs. , Nuclear graphite H 451, used previously in the United States for nuclear reactor graphite components, is no longer available. New nuclear graphite grades have been developed and are considered suitable candidates for new HTR reactor designs. To support the design and licensing of HTR core components within a commercial reactor, a complete properties database must be developed for these current grades of graphite. Quantitative data on in service material performance are required for the physical, mechanical, and thermal properties of each graphite grade, with a specific emphasis on data accounting for the life limiting effects of irradiation creep on key physical properties of the HTR candidate graphite grades. Further details on the research and development activities and associated rationale required to qualify nuclear grade graphite for use within the HTR are documented in the graphite technology research and development plan.

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High Temperature Reactor Research and Development Roadmap, Draft for Public Comment

Nuclear power provides clean, reliable energy, contributing about 20 percent of the electricity generated in the United States. It supplies approximately 60 percent of our non-greenhouse-gas emitting power, making it our nation’s single largest contributor of carbon-free electricity. This vital component of the U.S. energy portfolio avoids hundreds of millions of tons of carbon dioxide emissions each year and supports hundreds of thousands of U.S. jobs, and yet is facing unprecedented challenges. Complex market factors, falling alternative generation costs and lower electricity demand forecasts have made operating nuclear power plants uneconomical in some parts of the country. The industry is confronting premature shut downs, a lack of new plants in the pipeline, profound market challenges and intense financing requirements. However, none of these challenges reflect a reduced need for this reliable and clean source of baseload power. Our nation’s nuclear sector urgently needs to adjust to these challenges to ensure continued availability of this vital national energy resource. The Department of Energy and its national laboratories are aggressively working to revive, revitalize, and expand U.S. nuclear energy capacity. We are advancing nuclear energy technologies through targeted early-stage investments to ensure a strong domestic industry now and into the future. By leveraging public-private partnerships and the national laboratory system, we are developing an advanced nuclear infrastructure, encouraging a resilient supply chain, and promoting a strong nuclear pipeline. A key element of this effort is to support the recent and rapid expansion in innovative advanced reactor development already being led by the U.S. nuclear industry. Advanced reactors, particularly non-light water reactor concepts, offer the potential for significant improvements to safety, economics and environmental performance, to help sustain and expand the availability of nuclear power as a clean, reliable and secure power source for our nation. As part of this strategy, the Department of Energy commissioned the development of technology roadmaps for advanced non-light-water reactor concepts. The starting point for the roadmaps is the technical readiness assessment performed as part of an advanced test and demonstration reactor study released in 2016 [ ]. The roadmaps show the Research and Development (R&D) needed to support demonstration of advanced reactor concepts, for either engineering demonstration or commercial demonstration depending on concept maturity, by 2035. The starting point for the roadmaps is the technical readiness assessment performed as part of an advanced test and demonstration reactor study released in 2016. The roadmaps were developed based on a review of technical reports and vendor literature summarizing the technical maturity of each concept and the outstanding R&D needs. Tasks for specific systems were highlighted on the basis of time and resources needed to complete the tasks and the importance of the system to the performance of the reactor concept. The roadmaps are intended to be generic (i.e., not specific to a particular vendor’s design); however, features of the General Atomics Energy Multiplier Module were included to provide specific examples for illuminating needed R&D tasks to be conducted in support of demonstration in the near future.

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Nuclear Data Management and Analysis System Plan

The United States Department of Energy Advanced Reactor Technologies Program was formed in Fiscal Year 2015 and encompasses the Next Generation Nuclear Plant Project and Very High Temperature Reactor (VHTR) Program as they were known previously. The VHTR Program was created to support design and licensing of the first VHTR nuclear plant. Data created for and used by the program must be qualified for use, stored in a readily accessible electronic form, categorized to assure the correct data are used, and controlled to prevent data corruption or inadvertent changes. The Nuclear Data Management and Analysis System was designed to support the data needs of the VHTR Program, at the time and now the Advanced Reactor Technologies Program. Since its inception, use of the Nuclear Data Management and Analysis System has expanded to support additional projects and programs with similar requirements for control, analysis, and availability of large data sets.

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Status of the NGNP graphite creep experiments AGC-1 and AGC-2 irradiated in the advanced test reactor

The United States Department of Energy's Next Generation Nuclear Plant (NGNP) Program will be irradiating six nuclear graphite creep experiments in the Advanced Test Reactor (ATR) located at the Idaho National Laboratory (INL). The graphite experiments will be irradiated over the next six to eight years to support development of a graphite irradiation performance data base on the new nuclear grade graphites now available for use in high temperature gas reactors. The goals of the irradiation experiments are to obtain irradiation performance data, including irradiation creep, at different temperatures and loading conditions to support design of the next generation nuclear plant (NGNP) very high temperature gas reactor, as well as other future gas reactors. The experiments will each consist of a single capsule that will contain six peripheral stacks of graphite specimens, with half of the graphite specimens in each stack under a compressive load, while the other half of the specimens will not be subjected to a compressive load during irradiation. The six peripheral stacks will have three different compressive loads applied to the top half of three diametrically opposite pairs of specimen stacks, while a seventh stack will not have a compressive load. The specimens will be irradiated in an inert sweep gas atmosphere with on-line temperature and compressive load monitoring and control. There will also be sampling the sweep gas effluent to determine if any oxidation or off-gassing of the specimens occurs during irradiation of the experiment.

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PRELIMINARY RESULTS OF THE AGC-4 IRRADIATION IN THE ADVANCED TEST REACTOR AND DESIGN OF AGC-5 (HTR16-18469)

The United States Department of Energy’s Advanced Reactor Technologies (ART) Program will irradiate up to six nuclear graphite creep experiments in the Advanced Test Reactor (ATR) located at the Idaho National Laboratory (INL). The graphite experiments are being irradiated over an approximate eight year period to support development of a graphite irradiation performance data base on the new nuclear grade graphites now available for use in high temperature gas reactors. The goals of the irradiation experiments are to obtain irradiation performance data, including irradiation creep, at different temperatures and loading conditions to support design of the Very High Temperature Gas Reactor (VHTR), as well as other future gas reactors. The experiments each consist of a single capsule that contain six stacks of graphite specimens, with half of the graphite specimens in each stack under a compressive load, while the other half of the specimens are not be subjected to a compressive load during irradiation. The six stacks have differing compressive loads applied to the top half of diametrically opposite pairs of specimen stacks. A seventh specimen stack in the center of the capsule does not have a compressive load. The specimens are being irradiated in an inert sweep gas atmosphere with on-line temperature and compressive load monitoring and control. There are also samples taken of the sweep gas effluent to measure any oxidation or off-gassing of the specimens that may occur during initial start-up of the experiment. The first experiment, AGC-1, started its irradiation in September 2009, and the irradiation was completed in January 2011. The second experiment, AGC-2, started its irradiation in April 2011 and completed its irradiation in May 2012. The third experiment, AGC-3, started its irradiation in late November 2012 and completed in the April of 2014. AGC-4 is currently being irradiated in the ATR. This paper will briefly discuss the preliminary irradiation results of the AGC-4 experiment, as well as the design of AGC-5.

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Preliminary results of AGC-4 irradiation in the advanced test reactor and design of AGC-5 - 18469

The U.S. Department of Energy Advanced Reactor Technologies Program will irradiate up to six nuclear graphite creep experiments in Idaho National Laboratory Advanced Test Reactor (ATR). The graphite experiments are being irradiated over an approximate 8-year period to support development of a graphite irradiation performance database on new nuclear grade graphites now available for use in high-temperature gas reactors. The goals of the irradiation experiments are to obtain irradiation performance data, including irradiation creep, at different temperatures and loading conditions to support design of the very high-temperature gas reactor and other future gas reactors. Each of the experiments consist of a single capsule that contains six stacks of graphite specimens, with half of the graphite specimens in each stack under a compressive load and the other half of specimens not subjected to a compressive load during irradiation. The six stacks have differing compressive loads applied to the top half of the diametrically opposite pairs of specimen stacks. A seventh specimen stack in the center of the capsule does not have a compressive load. The specimens are being irradiated in an inert sweep gas atmosphere with online temperature and compressive load monitoring and control. Also, samples are taken of sweep gas effluent to measure any oxidation or off-gassing that may occur during initial startup of the experiment. The first experiment Advanced Graphite Capsule (AGCJ-I started irradiation in September 2009 and completed in January 2011; the second experiment AGC-2 started irradiation in April 2011 and completed in May 2012; the third experiment AGC-3 started irradiation in late November 2012 and completed in April 2014; and AGC-4 is currently being irradiated in ATR. This paper will briefly discuss preliminary irradiation results from the AGC-4 experiment and design of AGC-3. (authors)

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