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Investigation of temperature dependence of fracture toughness in high-dose HT9 steel using small-specimen reuse technique

The temperature dependence of fracture toughness in HT9 steel irradiated to 3–145 dpa at 380–503 degrees*C was investigated using miniature three-point bend (TPB) fracture specimens. A miniature-specimen reuse technique has been established: the tested halves of subsize Charpy impact specimens with dimensions of 27 mm *3mm* 4 mm were reused for this fracture test campaign by cutting a notch with a diamond-saw in the middle of each half, and by fatigue-precracking to generate a sharp crack tip. It was confirmed that the fracture toughness of HT9 steel in the dose range depends more strongly on the irradiation temperature than the irradiation dose. At an irradiation temperature <430 *degreesC, the fracture toughness of irradiated HT9 increased with the test temperature, reached an upper shelf of 180—200 MPa*m^.5 at 350–450 degrees*C, and then decreased with the test temperature. At an irradiation temperature >430 degrees*C, the fracture toughness was nearly unchanged up to about 450 *degreesC and decreased slowly with test temperatures in a higher temperature range. Such a rather monotonic test temperature dependence after high-temperature irradiation is similar to that observed for an archive material generally showing a higher degree of toughness. A brittle fracture without stable crack growth occurred in only a few specimens with relatively lower irradiation and test temperatures. In this discussion, these TPB fracture toughness data are compared with previously published data from 12.7 mm diameter disc compact tension (DCT) specimens.

Baek, Jong-Hyuk↗

Second Annual Progress Report on Correlation Between Microstructure and Mechanical Properties of Neutron-Irradiated Ferritic-Martensitic and Austenitic Steels

Ferritic-martensitic steels G92-2b (an optimized Grade 92 heat), NF616 and T91, and austenitic stainless steel 800H and its Grain Boundary Engineering (GBE)-treated version 800H-TMP (ThermoMechanical Processing) were irradiated in the High Flux Isotope Reactor (HFIR) of Oak Ridge National Laboratory (ORNL) and the Advanced Test Reactor (ATR) of Idaho National Laboratory (INL). Selected G92-2b samples were irradiated up to 14.66 dpa in the HFIR at two temperature ranges: 400–496.7°C and 683.3– 720°C. NF616 and T91 were irradiated in the ATR up to 8.16 dpa with the irradiation temperatures ranged from 241°C to 447.5°C. Alloy 800H and 800H-TMP samples were irradiated in both the HFIR and the ATR. Selected 800H and 800H-TMP samples had HFIR irradiation to 1.28 dpa at 580°C and ATR irradiation up to 9.12 dpa at 359°C to 431°C. Vickers hardness measurements, fractography, and microstructural characterization were performed on the selected samples in the Low Activation Materials Design and Analysis (LAMDA) laboratory. Radiation-hardening of G92-2b was observed at the lower doses and lower irradiation temperatures (400- 496.7°C), with GB03 (0.52 dpa at 400°C) and GB04 (7.44 dpa at ~490°C) showing ~12% and ~8% hardening, respectively. Softening by ~14% was observed for GB05 (14.66 dpa at 496.7°C). Radiationsoftening of G92-2b was more prevalent at the higher irradiation temperatures (683.3-~720°C), with GB10 (0.46 dpa at 683.3°C), GB11 (7.44 dpa at ~720°C), and GB12 (14.63 dpa at ~720°C) showing ~8%, ~8%, and ~40% softening, respectively. Radiation-hardening of NF616 and T91 was observed with the hardness increased by ~37% to ~65% depending on the irradiation doses and irradiation temperatures. Within the studied irradiation conditions of NF616 and T91, samples with a higher dose had a larger hardness after irradiation. All the tested alloy 800H and 800H-TMP samples in this work showed radiation-hardening by ~96±7% to ~152±10%. Alloy 800H-TMP tended to have slightly smaller radiation-hardening than alloy 800H. The fractography results of G92-2b sample GB03, GB10, and GB11, together with the previously characterized fractography of GB04, GB05, and GB12, indicated that the ductility of G92-2b was maintained up to 14.66 dpa at the lower irradiation temperatures of 400-496.7°C, while some loss of ductility (less necking) was observed for higher doses at the higher irradiation temperatures of 683.3-720°C. This agrees with the previously reported tensile test results of G92-2b, where the elongation of G92-2b was reduced at higher doses at the higher irradiation temperatures. Dimple sizes increased at higher doses, which are more evident at the higher irradiation temperatures of 683.3-~720°C. The fractography of NF616 sample D2 (2.96 dpa at 291.5°C), D4 (5.91 dpa at 359°C), and D6 (8.16 dpa at 431°C) indicated loss of ductility with negligible necking for sample D2, while ductile failure for samples D4 and D6. Fractography of alloy 800H and 800H-TMP samples in various irradiation conditions showed ductile failure with obvious necking. Dimples were observed, with some of them containing large Ti-rich particles, in all the 800H/800H-TMP samples. Electron backscatter diffraction characterization of GB12 indicated the recovery of the lath structure, which was generally replaced by an equiaxed grain structure. Transmission electron microscopy (TEM) characterization showed the presence of frequent M 23 C 6 (M = primarily Cr), MX (M = primarily V), spherical Nb(C,N) precipitates, and occasional Laves phase precipitates in the G92-2b samples. MX precipitates with sizes of 20-30 nm were observed at boundaries of smaller grains, indicating the pinning effect of the V-rich precipitates. The lath structure recovery was more evident at the higher irradiation temperatures (683.3-~720°C), with decreased densities of line dislocations and M23C6 precipitates. The irradiated T91 (TA04) showed the growth of M23C6 precipitates to 101 ± 40 nm from the initial 68 ± 22 nm in the unirradiated condition. Dislocation loops of both {100} and {111} types were present in TA04. TEM characterization was also performed on the irradiated 800H (N4, N5, N6, and AR2) and 800H-TMP (P4, P5, P6, and HG1). Accumulation of M 23 C 6 precipitates at grain boundaries was observed in all the xii 800H/800H-TMP samples, and the presence of Ti(C,N) precipitates at grain boundaries and in the matrix was observed in the irradiated 800H-TMP. Some Ti(C,N) precipitates are embedded in the M 23 C 6 precipitates, maintaining specific orientation relationships between the precipitates and between the precipitate and matrix. In addition, nanoscale Si-rich clusters were observed in the matrix of all the 800H/800H-TMP samples, with EDS Si maps tending to have a lower contrast in 800H-TMP samples. Atom probe tomography was conducted on the same samples, supported by a Rapid Turnaround Examination project under Nuclear Science User Facilities. The results are being analyzed to be integrated with the TEM results for a confident description of the γ’ precipitates. Dislocation loops also formed in all the 800H/800H-TMP samples. The density and the average size of dislocation loops were quantified to be in the order of 10 22 – 10 23 m -3 and 11.7 – 15.9 nm, respectively, in the ATR-irradiated 800H/800H-TMP samples. The loop densities in irradiated 800H were higher than that in irradiated 800H-TMP under the same irradiation conditions. Further systematic data analyses, together with some complementary experiments, will be pursued for these samples to foster peer-reviewed journal article publications.

36 MATERIALS SCIENCE↗

Fracture Toughness Characterization of Generation II FeCrAl Alloys after ~18 dpa Irradiation

FeCrAl alloys are promising candidate materials for the accident tolerant fuel (ATF) cladding applications due to their excellent corrosion resistance to the elevated temperature steam environment. Currently, the handbook on FeCrAl material properties contains only limited data regarding the fracture toughness properties of any FeCrAl alloy. This includes alloys currently under investigation within the Advanced Fuels Campaign (AFC) at Oak Ridge National Laboratory (ORNL). In this project, a series of irradiation capsules have been irradiated in the High Flux Isotope Reactor (HFIR) at ORNL with two Generation II FeCrAl candidate alloys, i.e., C06M and C36M, to assess the fracture response of these alloys after neutron irradiation. These alloys represent the “book-end” compositions for C26M, the alloy currently being developed as the leading candidate for LWR cladding. A total of six irradiation capsules were irradiated in HFIR at target temperatures of 200°C, 330°C, and 500°C up to target damage doses of 8 displacements per atom (dpa) and 16 dpa. These damage doses represent the expected middle and end of life damage levels for typical LWR cladding while the irradiation temperature regimes will provide insight into the role of varying microstructural features on the fracture toughness properties of neutron irradiated FeCrAl alloys. To date, irradiation of all capsules has been completed in HFIR. This report summarizes the latest results of microhardness and fracture toughness PIE for the 16 dpa capsules (FCAB2, FCAB4, and FCAB6), for which the measured irradiation conditions were: 204°C/17.6dpa, 343°C/18.3dpa, and 507°C/18.6dpa. The main conclusions of this study can be summarized as follows: 1) After the 204°C/17.6dpa irradiation, both C06M and C36M exhibited significant irradiation hardening and embrittlement 2) After the 343°C/18.3dpa irradiation, both C06M and C36M exhibited small irradiation hardening without irradiation embrittlement 3) After the 507°C/18.6dpa irradiation, both C06M and C36M exhibited irradiation softening without irradiation embrittlement 4) Comparing the microhardness and Master Curve reference temperature T 0q before and after neutron irradiation, we did not observe a linear correlation between the two parameters for both C06M and C36M. This should be mainly due to a flat response of the Master Curve reference temperature T 0q to the irradiations at 166-204°C and 315-343°C ranges 5) C06M showed a lower T 0q , meaning better toughness, than C36M at the unirradiated condition and such trend was kept even after neutron irradiation except for the 166-204°C irradiation where both materials had similar T 0q . 6) In terms of hardening and embrittlement, the irradiation effect on both C06M and C36M appeared to saturate after an irradiation dose of 7 dpa.

36 MATERIALS SCIENCE↗

Comparison of Ion and Neutron Irradiations to 3 dpa at 500 deg. C in Ferritic-Martensitic Alloys

The growing global demand for energy will increasingly call upon advanced nuclear fission reactors to supply safe and reliable electricity. The structural and fuel cladding components of these reactors will be subject to extreme conditions of irradiation damage up to several hundred displacements per atom (dpa) at temperatures as high as 700 deg. C. Ferritic-martensitic (F-M) steels are leading candidates for these challenging conditions due to their strength and dimensional stability under irradiation. In order to accelerate the process for evaluating F-M alloys, charged particles are increasingly being used to emulate neutron irradiations. Charged particle irradiations allow the possibility of conducting irradiation experiments within a shorter time period (i.e. at a rate up to 4 orders of magnitude faster) and with minimal radioactivation of the material, enabling lower cost and faster turnaround of post irradiation examination and analysis. However, the irradiation dose rate, damage cascade morphologies, and irradiation damage depth profiles all differ widely between protons, heavier ions, and neutrons. Currently, there is limited understanding of the significance of these physical differences and how they manifest in the irradiated microstructure and mechanical properties of F-M steels. The objective of this study is to evaluate charged particles as a surrogate for neutron irradiations in F-M alloys by assessing common irradiation conditions using Fe{sup ++} ions, protons, and neutrons. Keeping the temperature and dose consistent enables isolation of the effects of each irradiating particle and their respective dose rates and cascade morphologies. Specimens of HCM12A and HT9 were irradiated separately with protons, self-ions, and neutrons to a common dose of 3 dpa at 500 deg. C. The microstructure of each specimen was characterized with TEM and LEAP and compared to evaluate proton and self-ion irradiation as a surrogate for neutron irradiation at these conditions. - Proton, self-ion, and neutron irradiations produced consistent sizes and number densities of grains, carbides, dislocation lines, and dislocation loops. Voids were absent in all conditions. The charged particle irradiations have successfully reproduced the neutron irradiation results for these microstructural features without a temperature shift. - Nano-cluster evolution of Si-Mn-Ni-P and Cu-rich clusters was markedly different for each irradiating particle type. Some cluster morphology trends could be explained by differences in cascade volume for differing irradiating species. But dose rate likely also influences cluster evolution. - Cr-rich nanoclusters nucleated only in the neutron-irradiated HCM12A and HT9. This is likely due to thermal aging at 500 deg. C over a longer experimental time, as compared to the proton and self-ion irradiations. (authors)

36 MATERIALS SCIENCE↗

Post-Irradiation Fracture Toughness Characterization of Generation II FeCrAl Alloys

FeCrAl alloys are promising candidate materials for the accident tolerant fuel (ATF) cladding application due to their exceptional resistance to oxidation in elevated temperature steam environments. Currently, limited fracture toughness data are available for the FeCrAl alloys, including the FeCrAl alloys newly developed at Oak Ridge National Laboratory (ORNL) under the U.S. Department of Energy’s Advanced Fuels Campaign (AFC) program. In this study, two Generation II candidate FeCrAl alloys, i.e., C06M (81.8Fe-10Cr-6Al-0.03Y-2Mo-0.2Si) and C36M (78.8Fe-13Cr-6Al-0.03Y-2Mo-0.2Si), were irradiated in the High Flux Isotope Reactor (HFIR) at ORNL to assess the fracture characteristics of these alloys after neutron irradiation. A total of six rabbit capsules were irradiated in HFIR at target temperatures of 200°C, 330°C, and 500°C up to target damage doses of 8 displacements per atom (dpa) and 16 dpa. Post-irradiation fracture toughness testing was performed following the Master Curve method in the ASTM E1921 standard. The main findings of this study are:1) Both the C06M and C36M alloys exhibited a similar response to irradiation concerning irradiation hardening and embrittlement.2) The irradiation temperature played different roles in terms of irradiation hardening and embrittlement for both C06M and C36M: after irradiation between 166°C and 204°C, both materials exhibited significant irradiation hardening and embrittlement; after irradiation between 315°C and 343°C, both materials showed small irradiation hardening without irradiation embrittlement. After irradiation between 501°C and 507°C, however, the irradiation softening without irradiation embrittlement was observed in both materials.3) Comparing the microhardness and Master Curve reference temperature T0q before and after neutron irradiation, we did not observe a linear correlation between the two parameters for both C06M and C36M steels. This should be mainly due to a flat response of the Master Curve reference temperature T0q to the irradiations at 166–204°C and 315–343°C ranges4) C06M showed a lower T0q, meaning better toughness, than C36M at the unirradiated condition, and such trend was kept even after neutron irradiation except for the 166–204°C irradiation after which both materials had similar T0q.5) In terms of hardening and embrittlement, the irradiation effect on both C06M and C36M appeared to saturate after an irradiation dose of 7 dpa.

Chen, Xiang↗

Fundamental Studies of Irradiation-Induced Modifications in Microstructural Evolution and Mechanical Properties of Advanced Alloys

This final technical report summarizes the research performed during October 2014 and December 2017, with a focus on investigating the radiation-induced microstructural and mechanical property modifications in optimized advanced alloys for sodium-cooled fast reactor (SFR) structural applications. To accomplish these objectives, the radiation responses of several different advanced alloys, including austenitic steel Alloy 709 (A709) and 316H, and ferritic/ martensitic Fe–9Cr steels T91 and G92, were investigated using a combination of microstructure characterizations and nanoindentation measurements. Different types of irradiation, including ex situ bulk ion irradiation and in situ transmission electron microscopy (TEM) ion irradiation, were employed in this study. Radiation-induced dislocations, precipitates, and voids were characterized by TEM. Scanning transmission electron microscopy with energy dispersive X-ray spectroscopy (STEM-EDS) and/or atom probe tomography (APT) were used to study radiation-induced segregation and precipitation. Nanoindentation was used for hardness measurements to study irradiation hardening. Austenitic A709 and 316H was bulk-irradiated by 3.5 MeV Fe ++ ions to up to 150 peak dpa at 400, 500, and 600°. Compared to neutron-irradiated stainless steel (SS) 316, the Frank loop density of ion-irradiated A709 shows similar dose dependence at 400°, but very different temperature dependence. Due to the noticeable difference in the initial microstructure of A709 and 316H, no systematic comparison on the Frank loops in A709 vs 316H was made. It would be helpful that future ion irradiation study on 316 stainless steel could be conducted to directly compare the temperature dependence of Frank loop density in ion-irradiated 316 SS with that in neutron-irradiated 316 SS. In addition, future neutron irradiation on A709 at 400–600° at relative high dose (≥10 dpa) can be carried out to compare with ion-irradiated A709. The radiation-induced segregation (RIS) of Ni and Si was observed in both A709 and 316H in all irradiated conditions and was found at various sinks: line dislocations, dislocation loops, void surfaces, carbide-matrix interfaces, etc. Radiation also induced the formation of Ni,Si-rich precipitates. As suggested in a previous study on neutron-irradiated 316 stainless steel, one possible consequence of the significant RIS of Si is that the enrichment at defect sinks depletes the silicon in the matrix, which can lead to enhanced void nucleation rate. The enrichment of Ni and Si is accompanied by the depletion of Cr at defect sinks, which could also affect the corrosion resistance. Radiation-induced change in the orientation relationship of pre-existing MX precipitates was observed at 600°. It is believed that this change is associated with the network dislocations formed under irradiation. The underlying mechanism is still not well understood. This change could be a positive indication that the MX precipitates can survive high density network dislocations. It would be helpful if neutron irradiation at similar dose conditions could be carried out to verify that this effect is not unique for ion irradiation. Intragranular Cr-rich carbides with a core-shell structure, i.e. Cr-rich carbide core and Ni,Si-rich shell was found at 500° and 600° in the highest dose (150 peak dpa) specimens. Coarse voids (30 nm in diameter) were only commonly found at 500° in the 50 and 150 peak dpa specimens in regions less than 750 nm in depth. The highest swelling for A709 irradiated to 50 and 150 peak dpa at 500° is about 0.44% and 0.37%, respectively. Due to the choice of 100 degree temperature intervals, this study did not attempt to precisely identify peak void swelling conditions, merely the range of irradiation temperatures where this could be a concern. It is known high-dose ion irradiation can significantly suppress void nucleation. Future neutron irradiation in the 500–600° range (without considering the temperature shift) is needed to determine the onset of accelerated void swelling (possibly at lower dose).

36 MATERIALS SCIENCE↗

Unraveling Solar Wind Space Weathering of Carbon-Rich Asterods: Low-Flux VS. High-Flux Ion Irradiation of Murchison

Introduction: Space weathering processesalter the microstructural, compositional, and optical properties of airless planetary surfaces.Solar wind space weatheringforms ion-damaged rims within the outermost ~100 nm of regolith grains through atomic-displacements and implantation of energetic H+and He+ions[1]. Transmission electron microscope(TEM)studies of space weathered Itokawa and lunar olivine particles reveal predominantly nanocrystalline solar wind-damaged rims with only minor regions of amorphization[2-5]. This finding differs from laboratoryion irradiation experiments in which samples become amorphous at fluences 2-3 orders of magnitude lower than the independentlyconstrained fluences for still-crystalline natural samples [6-7].Ion flux is generally considered to have a secondaryeffectcompared to fluence in these irradiation experiments. However, solar wind irradiation of natural samples occurs at a flux that is ~4-5 orders of magnitude lower than whatisused inlaboratory simulations (e.g., [6,8-9]). Constraining how the very low ion flux of solar wind influences the microstructural, chemical, and spectral alteration of silicate minerals will improve our understanding of solar wind space weathering and aid in the analysis of returned samples from the Hayabusa2 and OSIRIS-REx missions. Here we report results from low-and high-flux ion irradiation experiments on the Murchison (CM2)meteoritewithcomparable total fluences. Methods: We performed low-flux and high-flux He+(4 keV) and H+(1 keV) irradiation experiments on separate, dry-cut Murchison slabs. Low-flux He+irradiation reached a total fluence of 2.1 x 1016ions/cm2(~400 years of exposure at Bennu) using a flux of 3.6 x 1011ions/cm2/s; low-flux H+irradiation reached a total fluence of 3.9 x 1016ions/cm2(~30 years) using a flux of 6.6 x 1011ions/cm2/s. High-flux He+irradiation reached a total fluence of 2.0 x 1016ions/cm2(~400 years)using a flux of 9.1 x 1012ions/cm2/s; high-flux H+irradiation reached a total fluence of 5.8 x 1016ions/cm2(~50 years)using flux of 8.4 x 1012ions/cm2/s. By irradiating to similar total fluences in both the low-flux and high-flux experiments, we can better isolate and evaluatethe effects of ion flux. Differences between unirradiatedand irradiated surfaces are determined using threeanalytical techniques:(1) in situX-ray photoelectron spectroscopy(XPS) reveals changes in surface chemistry,(2) visible to near-infrared spectroscopy (VNIR; 0.35-2.5 μm) highlights changes in spectraltrends, such as albedo and slope, and (3) TEM and energy-dispersive X-ray spectroscopy (EDS) identifieschanges in nanoscale structure and elemental composition within olivine and matrix electron-transparent thin sections prepared using focused ion beam scanning electron microscopy (FIB-SEM). Results and Discussion: XPS analyses of the low-fluxand high-fluxHe+-and H+-irradiated samples showa minorreduction in surface carbon contentand chemicalreduction ofFe3+to Fe2+. The latter result is consistent with the higher Fe2+/Fe3+ratios observed in phyllosilicate-rich space weathered rims of Ryugu grains [10].VNIR analyses suggest that the low-flux H+-irradiated spectrum has a slightly bluer slope (over 0.65-2.5 μm) compared to the unirradiated VNIR spectrum from [9] while the low-flux He+-irradiated spectral slope is comparable to the unirradiated surface. Both the high-flux He+-and H+-irradiated VNIR spectra exhibitslightlyhigheralbedos at shorter wavelengths relativeto their unirradiated counterparts, with He+irradiation yielding a greater change. Thus far, the low-flux He+-irradiated matrix and olivine FIBsections as well as the low-flux H+-irradiated olivine FIBsection have been examined with TEM. The surfaces of all three samplesshowless vesiculation than high-flux/high-fluenceirradiated matrix and olivine samples from [9]. The depth of phyllosilicate amorphization in thelow-fluxHe+-irradiated matrix FIBsection varieslaterally, with crystalline domains occurring as shallow as ~25 nm in some regions. Thelow-flux He+-irradiated olivine FIBsection has acontinuous,~40-90 nm thick ion-affected layer with polycrystalline and amorphous microstructures. The low-flux H+-irradiated olivine sampleexhibits a distinct, ~10-40 nm ion-affected layer whose uppermost ~20 nmin thicker regions is predominantly amorphous.Continuing to compare results from this work to those from [9] will provide a comprehensive understanding of how ion flux impacts the microstructural, chemical, and optical modification of various mineral phases and, in turn,help identify space weathering features from parent body alteration in Hayabusa2 and OSIRIS-REx returned samples.

D L Laczniak↗

In-situ ion irradiation of ZIRLO alloy

As an alternative to in-core neutron irradiations which are lengthy and costly, ex-core irradiations with energetic ions are envisioned as a possible way to probe the irradiation response of zirconium alloys used in pressurized water reactors (PWRs). Such ion irradiations, being well-controlled experiments, could offer a powerful, easier, and quicker way to study irradiation induced microstructural changes without remote handling that typically lead to structural component dimensional change (such as irradiation growth). Thus these irradiation experiments could help in the development of advanced dimensionally stable and deformation resistant alloys. For this matter, an initial investigation was performed to determine the feasibility of using ex-core ions to develop irradiation damage typically observed after neutron irradiation in Westinghouse's ZIRLO alloy. In-situ ion irradiations of ZIRLO alloy were conducted at the IVEM-Tandem Facility at Argonne National Laboratory at different dose levels and at different temperatures. The initial goal is to induce radiation damage of similar levels (in terms of dpa) to what develops during in-core neutron irradiation and analyze the potential of using ion irradiation as a substitute for in core neutron irradiation of Zr alloys. To facilitate comparison and convergence to in-core neutron irradiation, samples were ion irradiated in transmission and the amount of dpa developed during the ion irradiation was calculated using monte-Carlo based SRIM code. The TEM observations showed that the ion irradiation induced microstructure consisted of - and -type dislocation loops with the -loops developing at a later stage than the - loops, similarly to irradiation damage typically induced in neutron irradiated zirconium alloys. The study offers promises that heavy ion irradiation could potentially, under well-chosen conditions, be used to simulate neutron irradiation damage in PWRs. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Materials Irradiation Facility (MIF) at the High Flux Isotope Reactor (HFIR)

The Material Irradiation Facility (MIF) at the Oak Ridge National Laboratory (ORNIL) High Flux Isotope Reactor (HIFR) controls and monitors instrumented irradiation experiments for materials and fuel research. In 2013 ORNIL founded a Laboratory Directed Research and Development project to reinvigorate the use of instrumented experiments by redesigning MIF to enhance its capabilities. MIF improvements include an updated and more sophisticated experiment monitoring system, a modular design allowing easier addition of simultaneous experiments, and features that allow rapid incorporation of additional instrumentation Interest in materials and fuel irradiation has increased significantly over the last decade. Much of this interest is related to investigating the performance of advanced materials for fusion environments, designing and developing improved fuel and cladding materials, and examining material characteristics and behavior under irradiation conditions. At ORNL, the irradiation engineering team has more than 60 years of experience designing and fabricating various types of irradiation experiments. Rabbit capsule experiments are small scale and relatively inexpensive. These capsules are typically designed to be irradiated in the flux-trap region of the core. Full-length target capsules are larger scale and could be either instrumented or non-instrumented. These more complicated capsules can be irradiated in any of the experiment facilities at HFIR. Instrumented experiment irradiation provides significant advantages for researchers. The unique advantage is that the researcher can monitor and acquire in situ data and change capsule operating conditions in real time during the irradiation. This capability enables tight control of desired experimental conditions so that they match the design specifications throughout the irradiation. Also, the experiment conditions (e.g., temperature and pressure) can be altered during the test, enabling significant flexibility and the ability to collect considerably more data from a single experimental capsule. This capability allows measurement of a variety of material properties (conductivity, fission product composition, etc.) that otherwise would only be available upon post-irradiation examination, where non-equilibrium conditions brought on by irradiation do not exist. The data generated by these experiments contribute significantly to the understanding of material behavior under irradiation. MIF is an experimental platform that can host fully instrumented and monitored experiments in a high neutron flux environment. Its primary functions are to provide clean inert gas (helium, neon, argon) to experiments at controlled pressures and flows, monitor irradiation conditions (typically temperatures and pressures) during irradiation, and monitor effluent gases from experiments. This facility allows monitoring of chemical processes during a fueled irradiation, where this becomes important for detecting fuel failures. This paper reports the efforts towards reestablishing the value of HFIR for instrumented irradiation experiments and the improvements to MIF that ultimately reduce the costs of instrumented irradiation. This project advances ORNL materials capabilities to new levels by providing a state-of-the art, robust and flexible facility that can be expanded as customer requirements change, while supporting the goals of the fusion, advanced fuels, and structural materials programs. (authors)

42 ENGINEERING↗

Deciding Between an X-Ray and 137Cs Irradiator – It’s Not Just About Energy Spectra

Irradiators utilizing radioactive cesium-137 or cobalt-60 have been used for medical applications for many decades. This includes the irradiation of much of the nation’s blood supply, and radiation biology research. In 2005, the U.S. Nuclear Regulatory Commission was assigned to evaluate and prevent the misuse of radioactive materials with malicious intentions, with gamma-ray sources being high on the list. Licensees who possessed higher quantities of radioactive material of concern were required to set up increased security controls such as constant surveillance, controlled access, personnel background checks, and other security controls. As a result of introducing such regulations, and problems with disposing of high activity sources, many users of gamma-ray sources started to look into alternative technologies to replace their gamma-ray irradiators – the main alternative being an X-ray irradiator. To make an educated decision on whether a particular type of X-ray irradiator is equivalent to a particular type of cesium-137 irradiator for specific applications, one has to rely on relevant published comparison studies from other researchers, or perform the comparison studies on their own. This publication focuses on the authors’ technical performance comparison of two cesium-137 irradiator models and two X-ray irradiator models, for the purpose of determining whether the X-ray irradiator models could validly replace the cesium-137 irradiator models for certain applications. Utilizing 47 gram and 120 gram tissue-equivalent rodent dosimetry phantoms, our results indicate that, depending upon the user’s dose uncertainty budget and maximum size of specimens to be irradiated, the Model RS2000 160 kVp X-ray irradiator, Model XRAD-160 X-ray irradiator, or Model XRAD-320 X-ray irradiator, could successfully replace a cesium-137 irradiator. It is expected such equivalency could be extrapolated to other irradiated specimens of known sizes and density. Results also reveal that differences in inherent source geometry, field geometry and irradiation geometry can counter some of the influence due to differences in energy spectrum. It is hoped that this publication can be used as a guide for other similar studies, providing investigators guidance on important details that can make the difference between strong and weak comparison conclusions.

Cs-137 irradiator, X-ray Irradiator, self-containe↗

Discerning the effect of various irradiation modes on the corrosion of Zircaloy-4

Using proton irradiation, this study investigates the individual influence of several factors on the corrosion kinetics of Zircaloy-4 in a hydrogenated water environment simulating a Pressurized Water Reactor (PWR). Using both simultaneous irradiation-corrosion and autoclave corrosion, we separately examine: (i) the effect of pre-irradiation on modifying the structure of the material, (ii) the impact of irradiation on creating defects in the growing oxide layer during corrosion, and (iii) the influence of irradiation on increasing the corrosion potential through radiolysis during corrosion. To replicate neutron-irradiated microstructure, two proton pre-irradiation schedules were employed: Schedule 1 (isothermal irradiation at 350 °C to 5 dpa) to simulate high-temperature PWR conditions, and Schedule 2 (two-step process: irradiation to 2.5 dpa at -10 °C followed by 2.5 dpa at 350 °C) to simulate lower temperature PWR and Boiling Water Reactor (BWR) conditions. Long-term autoclave corrosion testing over 360 days at 320 °C revealed no significant difference between unirradiated samples and those pre-irradiated according to either schedule, with all samples exhibiting sub-cubic kinetics within the pre-transition regime. Irradiated samples underwent Simultaneous Irradiation Corrosion (SIC) tests, corroding in 320 °C water while being irradiated with protons. Corrosion was found to accelerate in all SIC-tested samples relative to autoclave conditions, with the greatest increase observed in non-pre-irradiated samples. Pre-irradiation with either schedule resulted in a slower corrosion rate compared to non-pre-irradiated regions under SIC conditions. The degree of radiolysis observed in the SIC tests surpassed typical PWR conditions, approaching levels found in BWRs. Radiolysis products were identified as the primary contributors to accelerated corrosion, corroborated by radiolysis bar tests. Furthermore, these findings underscore the intricate interactions between irradiation, corrosion, and water chemistry in determining Zircaloy-4 corrosion kinetics within nuclear reactor environments.

Pressurized Water Reactor↗

AGR-5/6/7 Irradiation Test Final As-run Report

This document presents the as-run analysis of the Advanced Gas Reactor (AGR) 5/6/7 irradiation experiment. AGR-5/6/7 is the last of a series of experiments conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) in support of the development and qualification of tri-structural isotropic (TRISO) low enriched fuel for use in high-temperature gas-cooled reactors (HTGR). The test train contained five separate capsules that were independently controlled and monitored. Each capsule contained multiple 24.91-mm-long and 12.25-mm-dimeter compacts filled with low-enriched uranium carbide/oxide tri-structural isotropic fuel particles. The objectives of the AGR 5/6/7 experiment were to: 1. Irradiate reference-design fuel particles to support fuel qualification. 2. Establish operating margins for the fuel, beyond normal operating conditions. 3. Provide irradiated-fuel performance data and irradiated-fuel samples for post irradiation examination and safety testing. The primary objective of the AGR-5/6 test (Capsules 1, 2, 4, and 5) was to verify the successful performance of the reference-design fuel under normal operating conditions. The AGR-7 test (Capsule 3) was designed to explore fuel performance at higher temperatures. Its primary objective is to demonstrate the capability of the fuel to withstand conditions beyond normal operating conditions, in support of plant design and licensing. AGR 5/6/7 will also provide irradiated-fuel performance data based on the fission gas release from particles during irradiation. To achieve the test objectives, the AGR-5/6/7 experiment was irradiated in the northeast (NE) flux trap of the ATR with a planned duration of 500 effective full-power days (EFPDs). The NE flux trap was selected because its larger diameter provided greater flexibility for test-train design compared to the Large B positions used for the AGR-1 and AGR-2 irradiations, significantly enhancing test capabilities for the combined irradiation campaigns. Due to delays in the ATR schedule, the AGR-5/6/7 irradiation was significantly shorter than the originally planned 13-cycle schedule. Irradiation began on February 16, 2018 and ended on July 22, 2020, spanning nine ATR cycles (162B?168A) over two and a half years. Thus, the AGR-5/6/7 fuel compacts were irradiated for a total of approximately 360.9 EFPDs. Final burnup values, on a per-compact basis, ranged from 5.66% to 15.26% fissions per initial heavy metal atom, while fast fluence values ranged from 1.62 to 5.55 × 1025 n/m2 (E >0.18 MeV). Time-averaged volume-averaged fuel temperatures on a capsule basis at the end of irradiation ranged from 756°C in Capsule 5 to 1313°C in Capsule 3 excluding days with significantly lower temperature during the two short powered axial locator mechanism cycles, 163A and 167A. By the end of irradiation, 48 out of 54 installed thermocouples (TC) had failed (the bottom three capsules lost all TCs). During the first five cycles (162B ? 165A), fission-gas isotope release-rate-to-birthrate (R/B) ratios were stable in the 10-8?10-6 range, and no in-pile particle failures were observed based on the gross gamma counts. During this time, the high exposed kernel fraction and high fuel particle temperatures in Capsule 1 led to the maximum R/B value of around 2 ? 10-6 for Kr-85m. The fission gas release in all capsules started to increase from the second half of Cycle 166A, when a large number of in-pile particle failures occurred in Capsule 1 and a gas line problem in this capsule caused fission gas leakage at various degrees into the other four capsules. This gas line problem also prevented fission gas release measurement for Capsule 1 during the last three cycles due to gas flow isolation. By the end of irradiation, it is estimated that approximately 15 particle failures in Capsule 3, which was considered possible at the start of the irradiation, since the experiment was designed to operate beyond the high-temperature gas-cooled reactor (HTGR) normal operating temperature range. A few hundred in-pile particle failures were estimated for Capsule 1 by the end of Cycle 166A, but the total number of failures is unknown due to lack of fission gas release data in the later cycles. Additionally, four potential in-pile failures were identified for Capsule 2 during the last cycle, 168A. In contrast, no in-pile failures were identified in the top two capsules (4 and 5) based on absence of the typical spikes in gross gamma counts and low failure estimates using the AGR-3/4 R/B per exposed kernel model.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Change of cell growth and mitochondrial membrane polarization in the progeny of cells surviving low-dose high-LET irradiation from Ra-226

Highlights: • Chronic low-dose high-LET α-radiation from Ra-226 is effective in inducing lethal mutations. • Decreased clonogenic survival did not occur in descendants of irradiated HaCaT survivors, and hormesis may be induced. • Mitochondrial membrane depolarization may be involved in the induction of lethal mutation. In order to test the delayed effect of radiation on the progeny of irradiated survivors, the human keratinocyte cell line HaCaT and the fish common bluegill embryonic cell line CHSE/F were exposed to low-dose high-LET α-radiation from Ra-226 or γ-rays. The clonogenic survival fraction, mitochondrial membrane polarization (MMP) and reproductive ability of the descendants of the surviving cells were measured. For progeny of irradiated HaCaT survivors, no delayed cell death occurred. On the contrary, progeny at about 47 cell doublings after Ra-226 irradiation and progeny at about 14 cell doublings after γ-irradiation showed increased clonogenic survival. However the total cell number was reduced for progeny of Ra-226-treated cells up to about 47 cell doublings after irradiation and for progeny of γ-irradiated cells up to about 28 doublings after irradiation, which means low reproductive ability had appeared. In addition, α-radiation from Ra-226 had greater impact on the MMP of the HaCaT progeny than γ-rays. MMP of progeny of Ra-226-treated cells decreased at 5 cell doublings after irradiation and increased dose-dependently at 19 cell doublings after treatment, and then decreased dose-dependently at 47 cell doublings, while there was no significant effect on MMP in progeny of γ irradiated cells. The progeny of Ra-226-irradiated CHSE/F survivors showed more serious damage than the offspring of γ-irradiated CHSE/F cells. Significant, dose-dependent delayed cell death occurred in progeny of surviving cells up to about 61 cell doublings after Ra-226 treatment, and the reproductive ability was also significantly reduced. But the MMP increased, which might be because of the increased removal of dead cells. For progeny of CHSE/F cells surviving γ-rays radiation, no significant change in clonogenic survival occurred, except for offspring of cells surviving low dose (0.1 Gy and 0.5 Gy) irradiation, which had higher survival than control up to about 28 cell doublings after irradiation. But the number of cells which were the progeny of γ-irradiated survivors decreased dose-dependently up to about 28 cell doublings after γ-irradiation.

61 RADIATION PROTECTION AND DOSIMETRY↗

AGC-2 Specimen Post Irradiation Data Package Report

This report documents results of the post-irradiation examination material property testing of the creep, control, and piggyback specimens from the irradiation creep capsule Advanced Graphite Creep (AGC)-2 are reported. This is the second of a series of six irradiation test trains planned as part of the AGC experiment to fully characterize the neutron irradiation effects and radiation creep behavior of current nuclear graphite grades. The AGC-2 capsule was irradiated in the Idaho National Laboratory Advanced Test Reactor at a nominal temperature of 600°C and to a peak dose of 5 dpa (displacements per atom). One-half of the creep specimens were subjected to mechanical stresses (an applied stress of either 13.8, 17.2, or 20.7 MPa) to induce irradiation creep. All post-irradiation testing and measurement results are reported with the exception of the irradiation mechanical strength testing, which is the last destructive testing stage of the irradiation testing program. Material property tests were conducted on specimens from 15 nuclear graphite grades using a similar loading configuration as the first AGC capsule (AGC-1) to provide easy comparison between the two capsules. However, AGC-2 contained an increased number of specimens (i.e., 487 total specimens irradiated) and replaced specimens of the minor grade 2020 with the newer grade 2114. The data reported include specimen dimensions for both stressed and unstressed specimens to establish the irradiation creep rates, mass and volume data necessary to derive density, elastic constants (Young’s modulus, shear modulus, and Poisson’s ratio) from ultrasonic time-of-flight velocity measurements, Young’s modulus from the fundamental frequency of vibration, electrical resistivity, and thermal diffusivity and thermal expansion data from 100–500°C. No data outliers were determined after all measurements were completed. A brief statistical analysis was performed on the irradiated data and a limited comparison between pre- and post-irradiation properties is presented. A more complete evaluation of trends in the material property changes, as well as irradiation-induced creep due to irradiation, temperature, and applied load on specimens will be discussed in later AGC-2 post-irradiation examination analysis reports.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

AGR-5/6/7 Irradiation Test Final As-run Report

This document presents the as-run analysis of the Advanced Gas Reactor (AGR)-5/6/7 irradiation experiment. AGR-5/6/7 is the last of a series of experiments conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory in support of the development and qualification of tri-structural isotropic low-enriched fuel for use in high-temperature gas-cooled reactors. The test train contained five separate capsules that were independently controlled and monitored. Each capsule contained multiple 24.91-mm-long and 12.25-mm-dimeter compacts filled with low-enriched uranium carbide/oxide tri-structural isotropic fuel particles. The objectives of the AGR-5/6/7 experiment were to: • Irradiate reference-design fuel particles to support fuel qualification. • Establish operating margins for the fuel, beyond normal operating conditions. • Provide irradiated-fuel performance data and irradiated-fuel samples for post-irradiation examination and safety testing. The primary objective of the AGR-5/6 test (Capsules 1, 2, 4, and 5) was to verify the successful performance of the reference-design fuel under normal operating conditions. The AGR-7 test (Capsule 3) was designed to explore fuel performance at higher temperatures. Its primary objective was to demonstrate the capability of the fuel to withstand conditions beyond normal operating conditions, in support of plant design and licensing. AGR-5/6/7 will also provide irradiated-fuel performance data based on the fission gas release from particles during irradiation. To achieve the test objectives, the AGR-5/6/7 experiment was irradiated in the northeast flux trap of the ATR with a planned duration of 500 effective full-power days. The northeast flux trap was selected because its larger diameter provided greater flexibility for test-train design compared to the Large B positions used for the AGR-1 and AGR-2 irradiations, significantly enhancing test capabilities for the combined irradiation campaigns. Due to delays in the ATR schedule, the AGR-5/6/7 irradiation was significantly shorter than the originally planned 13-cycle schedule. Irradiation began on February 16, 2018 and ended on July 22, 2020, spanning nine ATR cycles (162B–168A) over two and a half years. Thus, the AGR-5/6/7 fuel compacts were irradiated for a total of approximately 360.9 effective full-power days. Final burnup values, on a per-compact basis, ranged from 5.66 to 15.26% fissions per initial heavy metal atom, while fast fluence values ranged from 1.62 to 5.55 × 1025 n/m2 (E >0.18 MeV). Time-averaged volume-averaged fuel temperatures on a capsule basis at the end of irradiation ranged from 756°C in Capsule 5 to 1313°C in Capsule 3 excluding days with significantly lower temperature during the two short powered axial locator mechanism cycles, 163A and 167A. By the end of irradiation, 48 out of 54 installed thermocouples had failed (the bottom three capsules lost all thermocouples). During the first five cycles (162B – 165A), the fission-gas isotope release-rate-to-birthrate (R/B) ratios were stable in the 10-8–10-6 range, and no in-pile particle failures were observed based on the gross gamma counts. During this time, the high exposed kernel fraction and high fuel particle temperatures in Capsule 1 led to a maximum R/B value of around 2 ? 10-6 for Kr-85m. The fission gas release in all capsules started to increase from the second half of Cycle 166A, when a large number of in-pile particle failures occurred in Capsule 1 and a gas line problem in this capsule caused fission gas leakage at various degrees into the other four capsules. This gas line problem also prevented a fission gas release measurement for Capsule 1 during the last three cycles due to gas flow isolation. By the end of irradiation, it is estimated that approximately 15 particles failed in Capsule 3, which was considered possible because the experiment was designed to operate beyond the high-temperature gas-cooled reactor normal operating temperature range. A few hundred in-pile particle failures were estimated for Capsule 1 by the end of Cycle 166A, but the total number of failures is unknown due to the lack of fission gas release data in the later cycles. Additionally, four potential in-pile failures were identified for Capsule 2 during the last cycle, Cycle 168A. In contrast, no in-pile failures were identified in the top two capsules (4 and 5) based on the absence of the typical spikes in gross gamma counts and low failure estimates using the AGR-3/4 R/B per exposed kernel model.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Early Energetic Particle Irradiation of the HED Parent Body Regolith

Previous studies have shown that many individual grains within the dark phase of the Kapoeta howardite were irradiated with energetic particles while residing on the surface of the early HED regolith. Particle tracks in these grains vary in density by more than an order of magnitude and undoubtedly were formed by energetic heavy (Fe) ions associated with early solar flares. Early Irradiation of HED Regolith: Concentrations of excess Ne alone are not sufficient to decide between competing galactic and solar irradiation models. However, from recent studies of depth samples of oriented lunar rocks, we have shown that the cosmogenic 21-Ne/22-Ne ratio produced in feldspar differs substantially between Galactic Cosmic Radiation (GCR) and solar protons, and that this difference is exactly that predicted from cross-section data. Using Ne literature data and new isotopic data we obtained on acid-etched, separated feldspar from both the light and dark phases of Kapoeta, we derive 21-Ne/22-Ne = 0.80 for the recent GCR irradiation and 21-Ne/22-Ne = 0.68 for the early regolith irradiation. This derived ratio indicates that the early Ne production in the regolith occurred by both galactic and solar protons. If we adopt a likely one-component regolith model in which all grains were exposed to galactic protons but individual grains had variable exposure to solar protons, we estimate that this early GCR irradiation lasted for about 3-6 m.y. More complex two-component regolith models involving separate solar and galactic irradiation would permit this GCR age to be longer. Higher-energy solar protons would permit the GCR to be longer. Higher-energy solar protons would permit the GCR age to be shorter. Further, cosmogenic 126(Xe) in Kapoeta dark is no more than a factor of about 2 higher than that observed in Kapoeta light. Because 126(Xe) can only be formed by galactic protons and not solar protons, these data support a short GCR irradiation for the HED regolith. This would also be the maximum time peRiod for the solar irradiation. Various asteroidal regolith models, based on Monte Carlo modeling of impact rates as a function of size and on irradiation features of meteorites, predict surface exposure times of about 0.1 to 10 m.y., and depend on such factors as gravity, rock mechanical properties, and micrometeoroid flux. Because the depth at which solar Fe tracks are produced (is much less than 1 micrometer) is much less than the depth at which Solar Cosmic Rays (SCR) Ne is produced (about 1 cm), for a reasonably well-stirred HED regolith the "surface exposure time" for SCR 21-Ne production should be significantly longer than that for solar tracks and some other surface irradiation features. Enhanced Solar Proton Irradiation: For bulk samples of Kapoeta dark feldspar and a one-component regolith model, the derived ratio of 21-Ne/22-Ne = 0.68 implies that the early production ratio of SCR 21-Ne to GCR 21-Ne was about 0.5-1.5. This ratio is independent of any assumptions about the fraction of dark grains that are irradiated or of the variability in the degree of solar irradiation among grains. The 21-Ne SCR/GCR ratio indirectly derived from bulk Kapoeta pyroxene is somewhat larger, as is the ratio derived for simple two-component regolith models. Individual feldspar grains that were extensively solar irradiated would require even larger 21-Ne SCR/GCR production ratios. In contrast, the theoretical SCR/GCR production ratio for lunar feldspar with 0 g/CM2 shield ing is is less than or equal to 2, and the lowest ratio observed in near-surface samples of lunar anorthosites is less than or equal to 1. Considering the greater solar distance of Vesta (compared to the Moon), the likelihood that SCR 21-Ne was acquired under some shielding where production rates are lower, and the likelihood that the exposure time to galactic protons exceeded the exposure time to solar protons because of their very different penetration depths, the 21-Ne SCR/GCR production ratio on the HED parent body was probably < 0.1. The relatively large difference between the derived 21-Ne SCR/GCR ratio in Kapoeta dark feldspar and the estimated production ratio strongly indicates that the early solar irradiation involved a flux -20-50x the recent solar flux. This enhanced proton flux was probably associated with an overall greater solar activity in the first approximately 10(exp 7) to 10(exp 8) years of solar history.

Bogard, D. D.↗