Stressed capsules of austenitic and martensitic steels irradiated in SINQ Target-4 in contact with liquid lead-bismuth eutectic

In the MEGAPIE target, the steels used for the proton beam entrance window and other components in the spallation reaction zone suffer not only from the irradiation damage produced by protons and neutrons but also from the corrosion and embrittlement induced by liquid lead-bismuth eutectic (LBE). Although these effects have been separately studied by a number of authors, the synergistic effects of irradiation, LBE corrosion and embrittlement are little understood. This work presents detailed analyses of two stressed capsules made of the austenitic steel EC316LN and the martensitic steel 9Cr2WVTa, which were irradiated in SINQ Target-4 in contact with LBE at calculated temperatures of 315 and 225 °C, respectively. The Electron Probe Microanalysis (EPMA) on the cross-sections of the capsules showed that the stagnant LBE induced only slight corrosion on both capsules and no cracks existed in the wall of the EC316LN capsule. Some cracks were observed in the electron beam weld (EBW) and its vicinity of the 9Cr2WVTa capsule, which can be attributed to the high stress inside the wall, the hardening of the material induced by either welding (without re-tempering) or irradiation, and the effects of LBE embrittlement.     

Temperature evaluation of an instrumented capsule after material irradiation tests in HANARO

An instrumented capsule has been used for an irradiation test of various nuclear materials in the research reactor, HANARO. The capsule is designed to have a standard 4-hole structure for the economical test of an RPV material at 290 ± 10 °C. The temperature of the specimens for the reactor powers, 0-24 MW, is measured by 12 thermocouples, and finite element (FE) analyses are also performed to compare and verify the irradiation test results. As a result of the tests and analyses, the maximum temperature at the reactor power of 24 MW is 256 °C for an irradiation test and 202.6 °C for an FE analysis at Stage 3 of the capsule. Also, for each stage of the capsule, the temperature difference of the specimen in the axial direction is very small to within 10 °C. It is expected that the results presented in this paper will be useful when designing the instrumented capsules for an irradiation test.     

Irradiation of structural materials in contact with lead bismuth eutectic in the high flux reactor

In the framework of the materials domain DEMETRA in the European Transmutation research and development project EUROTRANS, irradiation experiment IBIS has been performed in the High Flux Reactor in Petten. The objective was to investigate the synergystic effects of irradiation and lead bismuth eutectic exposure on the mechanical properties of structural materials and welds. In this experiment ferritic martensitic 9 Cr steel, austenitic 316L stainless steel and their welds have been irradiated for 250 Full Power Days up to a dose level of 2 dpa. Irradiation temperatures have been kept constant at 300 °C and 500 °C.During the post-irradiation test phase, tensile tests performed on the specimens irradiated at 300 °C have shown that the irradiation hardening of ferritic martensitic 9 Cr steel at 1.3 dpa is 254 MPa, which is in line with the irradiation hardening obtained for ferritic martensitic Eurofer97 steel investigated in the fusion program. This result indicates that no LBE interaction at this irradiation temperature is present. A visual inspection is performed on the specimens irradiated in contact with LBE at 500 °C and have shown blackening on the surface of the specimens and remains of LBE that makes a special cleaning procedure necessary before post-irradiation mechanical testing.     

Behavior of ferritic/martensitic steels after n-irradiation at 200 and 300 °C

High chromium ferritic/martensitic (F/M) steels are considered as the most promising structural materials for accelerator driven systems (ADS). One drawback that needs to be quantified is the significant hardening and embrittlement caused by neutron irradiation at low temperatures with production of spallation elements. In this paper irradiation effects on the mechanical properties of F/M steels have been studied and comparisons are provided between two ferritic/martensitic steels, namely T91 and EUROFER97. Both materials have been irradiated in the BR2 reactor of SCK-CEN/Mol at 300 °C up to doses ranging from 0.06 to 1.5 dpa. Tensile tests results obtained between −160 °C and 300 °C clearly show irradiation hardening (increase of yield and ultimate tensile strengths), as well as reduction of uniform and total elongation. Irradiation effects for EUROFER97 starting from 0.6 dpa are more pronounced compared to T91, showing a significant decrease in work hardening. The results are compared to our latest data that were obtained within a previous program (SPIRE), where T91 had also been irradiated in BR2 at 200 °C (up to 2.6 dpa), and tested between −170 °C and 300 °C. Irradiation effects at lower irradiation temperatures are more significant.     

Experimental verification of thermal decomposition of lead polonide

The chemical form of polonium in lead–bismuth eutectic (LBE) is an important issue, considering the problem of polonium contamination in nuclear systems that use LBE as a coolant and/or an irradiation target. It has been thought that polonium exists as lead polonide in LBE. Polonium forms compounds with several metals, some of which decompose at high temperatures. Thermal decomposition of lead polonide was not confirmed experimentally, but the temperature of decomposition was foreseen to be around 600 °C. In this paper, the thermal decomposition of lead polonide and its decomposition temperature were confirmed using neutron-irradiated LBE. Neutron-irradiated LBE ingots containing polonium-210 were heated at temperatures of 550 ± 10 °C or 630 ± 10 °C in a vacuum. Polonium, lead and bismuth evaporated from the LBE ingots, and were deposited onto the surface of type 316 stainless steel (316SS) plates at various controlled temperatures between 220 ± 20 °C and 450 ± 20 °C. After heating, the number of alpha particles emitted from polonium-210 deposited on 316SS plates was measured. The experimental results showed a clear difference in the alpha particle count rate, which indicated that lead polonide decomposed at a temperature between 550 ± 10 °C and 630 ± 10 °C.     

Radiation stability of prototype ITER-type resistive bolometers with improved electrical contacts

We present the results for reactor irradiation of prototype ITER-compatible resistive radiation hardened bolometers up to a total dose of ∼0.01 dpa (thermal/fast [E > 0.1 MeV] neutron fluence of 5.2/0.8 ×10¹⁹ n/cm²). The prototype bolometer has a 100 nm thick Pt meander deposited on an alumina ceramic substrate. Connection of the delicate meander with external wiring is provided via special binding posts placed on the substrate. The binding post consist of a Pt ring attached to the substrate using melted glass, with a laser welded 0.1 mm diameter Pt wire. A vacuum capsule with a special bolometer holder was designed and fabricated to allow reactor irradiation at ∼400 °C in vacuum. The desired temperature was obtained by balancing the radiation heat generation and thermal energy losses via radiation and conductive heat transfer. The resistance of the Pt meander was measured in the course of 19 days irradiation in the BR2 material testing reactor of the SCK·CEN. Immediately after insertion of the bolometer into the reactor a significant decrease of the meander resistance was observed. The resistance then stabilized after several days of irradiation. The meander resistance measurements were stable during the first week of irradiation, but then the electrical contact was lost. Post-irradiation inspection showed that the binding posts remained attached to the substrate while one of the Pt wires detached from the Pt ring most probably due to a bad laser weld.     

Compatibility of ferritic-martensitic steel T91 welds with liquid lead-bismuth eutectic: Comparison between TIG and EB welds

The 9 wt.% chromium ferritic-martensitic steel T91 is being considered as candidate structural material for a future experimental accelerator driven system (XT-ADS). This material and its welded connections would need to be used in contact with liquid lead-bismuth eutectic (LBE), under high irradiation doses. Both unirradiated tungsten inert gas (TIG) and electron beam (EB) welds of T91 have been examined by means of metallography, scanning electron microscopy (SEM-EDX), transmission electron microscopy (TEM), Vickers hardness measurements and tensile testing in both gas and liquid lead-bismuth environment. The TIG weld was commercially produced and post weld heat treated by a certified welding company while the post weld heat treatment of the experimental EB weld was optimized in terms of the Vickers hardness profile across the welded joint. The mechanical properties of the T91 TIG and EB welds in contact with LBE have been examined using slow strain rate tensile testing (SSRT) in LBE at 350 °C. All welds showed good mechanical behaviour in gas environment but total elongation was strongly reduced due to liquid metal embrittlement (LME) when tested in liquid lead-bismuth eutectic environment. The reduction in total elongation due to LME was larger for the commercially TIG welded joint than for the EB welded joint.     

Corrosion experiments and materials developed for the Japanese HLM systems

The static corrosion tests in lead-bismuth eutectic (LBE) were conducted from 450 °C to 600 °C to understand corrosion behavior and develop corrosion resistant materials for heavy liquid metal systems. While increase of Cr content in steels enhances corrosion resistance in LBE, the effect approaches a constant value above 12 wt% of Cr. Corrosion depth in LBE increases with increasing temperature and corrosion attack becomes severe above 550 °C even under the condition of high oxygen concentration. Nickel dissolution and Pb-Bi penetration occur in 316SS and JPCA above 550 °C under the condition of high oxygen concentration. When oxygen concentration decreases below the level of Fe oxide formation, corrosion attack on these steels also becomes violent due to dissolution of various elements and grain boundary corrosion. Whereas additions of 1.5 wt% Si to T91 and 2.5 wt% Si to 316SS improve corrosion resistance, the effect is insufficient taking fluctuation of oxygen concentration in LBE into consideration. Furthermore, addition of 1.5 wt% Si to T91 causes rise in DBTT. A new coating method using Al, Ti and Fe powders produces corrosion resistant coating layers on 316SS. The coating layers containing 6-8 wt% Al exhibit good corrosion resistance at 550 °C for 3000 h in LBE containing 10⁻⁶-10⁻⁴ wt% of oxygen.     

PbBi-cooled direct contact boiling water small reactor

A design concept of PbBi cooled direct contact boiling water small fast reactor (PBWFR) has been formulated with some design parameters identified. Water is injected into hot PbBi above the core, and direct contact boiling takes place in chimneys. Boiling bubbles rise due to buoyancy effects, which works as a lift pump for PbBi circulation. The generated steam passes through separators and dryers for the removal of PbBi droplets, and then flows into turbines for the generation of electricity. The system pressure of 7 MPa is as the same as that of the conventional boiling water reactors (BWRs). The outlet steam is superheated by 10°C to avoid the accumulation of condensate on a PbBi free surface in the reactor vessel. The control rods are inserted from above, which is different from the original concept. This insertion was chosen since the seal of steam at the top of the reactor vessel is technically much easier than the seal of PbBi at the bottom of the reactor vessel. The electric power of 150 MWe may be the maximum which is practically possible as a small reactor with economic competitiveness to conventional LWRs. A two-region core is designed. A decrease in reactivity was estimated to be 1.5%dk/kk′ for 15 years. A fuel assembly has 271 fuel rods with 12.0 mm in diameter and 15.9 mm in pitch in a hexagonal wrapper tube. The design limit of cladding temperature is specified to be 650°C for compatibility of cladding material with PbBi. As a result, the PbBi core outlet temperature becomes 460°C. The PbBi temperature rise in the core is 150°C. The conditions of the secondary coolant steam are as the same as those of conventional BWRs with thermal efficiency of 33%. The core is designed to have the breeding ratio of 1.1 and the refueling interval of 15 years as a reactor with a long-life core. Direct heat exchangers (DHX), reactor vessel air cooling systems (RVACS) and guard vessel are designed.     

Liquid Pb-Bi embrittlement effects on the T91 steel after different heat treatments

The present work aims to investigate the susceptibility of ferritic/martensitic steels of different strength to the embrittlement of liquid Pb-Bi eutectic (LBE). Slow strain rate tensile (SSRT) tests on specimens of the T91 steel in three tempering conditions at 500, 600 and 760 °C were conducted in Ar and in LBE at temperatures between 150 and 500 °C. For the specimens tempered at 760 °C (the normal tempering condition) the susceptibility of the steel to LBE embrittlement appeared at temperatures between 300 and 450 °C. With increasing the strength of specimens by lowering the tempering temperature, specimens tempered at 600 and 500 °C demonstrated more pronounced embrittlement effects, reflected by wider and deeper ‘ductility-troughs’. The results suggest that ferritic/martensitic steels with higher strength are more susceptible to LBE embrittlement. The LBE embrittlement effects can be attributed to the decrease of fracture stress resulted from the ‘weakening inter-atomic bond’ by LBE contacting at crack tips.     

A model for fission gas release and gaseous swelling of the uranium dioxide fuel coupled with the FALCON code

A comprehensive model GRSW-A was developed to analyse the processes of fission gas release, gaseous swelling and microstructural evolutions in the uranium dioxide fuel during base irradiation and under transient conditions. The GRSW-A analysis incorporates a number of models published in open literature, as well as some original models that were already published by the authors elsewhere. Consequently, only the most prominent aspects of GRSW-A and its coupling with the FALCON fuel behaviour analysis and licensing code are described in this paper. The analysis of fuel behaviour in the REGATE experiment is presented, which includes the base irradiation of the fuel segment in a PWR to a burn-up of about 50 MWd/kgU, which was followed by a power ramp in the SILOE research reactor. Besides, the generalized data on fission gas release (FGR) in PWR fuel during the base irradiation up to a burn-up of about 70 MWd/kgU is interpreted using coupled FALCON and GRSW-A. Moreover, a mechanistic interpretation of the published data for pellet swelling during the base irradiation up to a burn-up of 100 MWd/kgU is put forward. In all the cases, the coupled FALCON/GRSW-A analysis has shown the improved prediction capability compared to the original FALCON MOD01, which is achieved due to the account for the mutual effect of thermal and, in particular, high-burn-up-assisted mechanisms of fission gas release and swelling under steady-state and transient conditions.     

Influence of liquid lead and lead-bismuth eutectic on tensile, fatigue and creep properties of ferritic/martensitic and austenitic steels for transmutation systems

In this paper, the tensile, fatigue and creep properties of the Ferritic/Martensitic (F/M) steel T91 and of the Austenitic Stainless (AS) Steel 316L in lead-bismuth eutectic (LBE) or lead, obtained in the different organizations participating to the EUROTRANS-DEMETRA project are reviewed. The results show a remarkable consistency, referring to the variety of metallurgical and surface state conditions studied. Liquid Metal Embrittlement (LME) effects are shown, remarkable on heat-treated hardened T91 and also on corroded T91 after long-term exposure to low oxygen containing Liquid Metal (LM), but hardly visible on passive or oxidized smooth T91 specimens. For T91, the ductility trough was estimated, starting just above the melting point of the embrittler (T_M,E = 123.5 °C for LBE, 327 °C for lead) with the ductility recovery found at 425 °C. LME effects are weaker on 316L AS steel. Liquid Metal Assisted Creep (LMAC) effects are reported for the T91/LBE system at 550 °C, and for the T91/lead system at 525 °C. Today, if the study of the LME effects on T91 and 316L in LBE or lead can be considered well documented, in contrast, complementary investigations are necessary in order to quantify the LMAC effects in these systems, and determine rigorously the threshold creep conditions.     

Nano-cavities observed in a 316SS PWR flux thimble tube irradiated to 33 and 70 dpa

The radiation-induced microstructure of a cold-worked 316SS flux thimble tube from an operating pressurized water reactor (PWR) was examined. Two irradiated conditions, 33 dpa at 290 °C and 70 dpa at 315 °C were examined by transmission electron microscopy. The original dislocation network had completely disappeared and was replaced by fine dispersions of Frank loops and small nano-cavities at high densities. The latter appear to be bubbles containing high levels of helium and hydrogen. An enhanced distribution of these nano-cavities was found at grain boundaries and may play a role in the increased susceptibility of the irradiated 316SS to intergranular failure of specimens from this tube during post-irradiation slow strain rate testing in PWR water conditions.     

Radiation-damage in molybdenum-rhenium alloys for space reactor applications

Various Mo-Re alloys are attractive candidates for use as fuel cladding and core structural materials in spacecraft reactor applications. Molybdenum alloys with rhenium contents of 41-47.5% (wt%), in particular, have good creep resistance and ductility in both base metal and weldments. However, irradiation-induced changes such as transmutation and radiation-induced segregation could lead to precipitation and, ultimately, radiation-induced embrittlement. The objective of this work is to evaluate the performance of Mo-41Re and Mo-47.5Re after irradiation at space reactor relevant temperatures. Tensile specimens of Mo-41Re and Mo-47.5Re alloys were irradiated to ∼0.7 displacements per atom (dpa) at 1073, 1223, and 1373 K and ∼1.4 dpa at 1073 K in the High Flux Isotope Reactor at Oak Ridge National Laboratory. Following irradiation, the specimens were strained to failure at a rate of 1 × 10⁻³ s⁻¹ in vacuum at the irradiation temperature. In addition, unirradiated specimens and specimens aged for 1100 h at each irradiation temperature were also tested. Fracture mode of the tensile specimens was determined. The tensile tests and fractography showed severe embrittlement and IG failure with increasing temperatures above 1100 K, even at the lowest fluence. This high temperature embrittlement is likely the result of irradiation-induced changes such as transmutation and radiation-induced segregation. These factors could lead to precipitation and, ultimately, radiation-induced embrittlement. The objective of this work is to examine the irradiation-induced degradation for these Mo-Re alloys under neutron irradiation.     

Materials researches at the Paul Scherrer Institute for developing high power spallation targets

For the R&D of high power spallation targets, one of the key issues is understanding the behavior of structural materials in the severe irradiation environments in spallation targets. At PSI, several experiments have been conducted using the targets of the Swiss spallation neutron source (SINQ) for studying radiation damage effects induced by high energy protons and spallation neutrons. As well, experiments have been performed to investigate liquid lead-bismuth eutectic (LBE) corrosion and embrittlement effects on T91 steel under irradiation with 72 MeV protons. In this paper, an overview will be given showing a selection of results from these experiments, which include the mechanical properties and microstructure of ferritic/maretensitic (FM) steels (T91, F82H, Optifer etc.) and austenitic steels (EC316LN, SS 316L, JPCA etc.) irradiated to doses higher than ever attained by irradiation in a spallation environment, and the behaviors of T91 irradiated with 72 MeV protons in contact with flowing LBE.     

High temperature irradiation effects in selected Generation IV structural alloys

In the Generation IV Materials Program cross-cutting task, irradiation and testing were carried out to address the issue of high temperature irradiation effects with selected current and potential candidate metallic alloys. The materials tested were (1) a high-nickel iron-base alloy (Alloy 800H); (2) a nickel-base alloy (Alloy 617); (3) two advanced nano-structured ferritic alloys (designated 14YWT and 14WT); and (4) a commercial ferritic-martensitic steel (annealed 9Cr-1MoV). Small tensile specimens were irradiated in rabbit capsules in the High-Flux Isotope Reactor at temperatures from about 550 to 700 °C and to irradiation doses in the range 1.2-1.6 dpa. The Alloy 800H and Alloy 617 exhibited significant hardening after irradiation at 580 °C; some hardening occurred at 660 °C as well, but the 800H showed extremely low tensile elongations when tested at 700 °C. Notably, the grain boundary engineered 800H exhibited even greater hardening at 580 °C and retained a high amount of ductility. Irradiation effects on the two nano-structured ferritic alloys and the annealed 9Cr-1MoV were relatively slight at this low dose.     

Low cycle fatigue tests of surface modified T91 steel in 10 wt% oxygen containing Pb45Bi55 at 550 °C

Low cycle fatigue tests in air and LBE containing 10⁻⁶ wt% dissolved oxygen were conducted with T91 steel at 550 °C. T91 was employed in two modifications, one in the as-received state, and the other after alloying FeCrAlY into the surface by pulsed electron beam treatment (GESA process). Tests were carried out with symmetrical cycling (R = −1) with a frequency of 0.5 Hz and a total elongation Δε_t/2 between 0.3% and 2%. No influence from LBE on fatigue could be detected. Results in air and LBE showed similar behaviour. Additionally, no difference was observed between surface treated and none treated T91 specimens.     

Experimental study of swelling of irradiated solid methane during annealing

Solid methane is still widely in use at pulsed neutron sources due to its excellent neutronic performance (IPNS, KENS, Second Target Station at ISIS), notwithstanding poor radiation properties. One of the specific problems is radiolytic hydrogen gas pressure on the walls of a methane chamber during annealing of methane. In this paper results of an experimental study of this phenomenon under fast neutron irradiation with the help of a specially made low temperature irradiation rig at the IBR-2 pulsed reactor are presented. The peak pressure on the wall of the experimental capsule during heating of a sample irradiated at 23-35 K appears to have a maximum of 2.7 MPa at an absorbed dose 20 MGy and then falls down with higher doses. The pressure always reached its peak value at the temperature range 72-79 K. Generally, three phases of methane swelling during heating can be distinguished, each characterized by a proper rate and intensity.     

Influence of post irradiation annealing on the mechanical properties and defect structure of AISI 304 steel

The effect of post irradiation annealing on the mechanical properties and the radiation induced defect structure was investigated on stainless steel, of type AISI 304, that was irradiated up to 24 dpa in the decommissioned Chooz A reactor. The material was investigated both in the as-irradiated state as well as after post irradiation annealing. In the as-irradiated specimen the typical radiation induced defects were found as well as γ′-precipitates (Ni₃Si). Annealing at 400 °C had almost no effect on the radiation induced defects, but annealing at 500 °C resulted in the immediate unfaulting of the Frank loops. As to the mechanical properties, annealing at 400 °C did not strongly affect the yield strength and the ductility of the material, although the fraction of intergranular fracture during slow strain rate tensile tests under pressurised water reactor conditions, was significantly reduced. Annealing at 500 °C did reduce the yield strength and restored substantially the ductility and the strain hardening capability of the material. The microstructure investigated by transmission electron microscopy correlates to the mechanical test results. It was found that the observed defect changes after post irradiation annealing provide a reasonable explanation for the observed changes of the mechanical properties.