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.     

Tensile properties of EC316LN irradiated in SINQ to 20 dpa

The wide application of 316-type austenitic stainless steels in existing spallation targets requires a comprehensive understanding of their behavior in spallation irradiation environments. In the present study, EC316LN specimens were irradiated in SINQ targets to doses between 3 and 17.3 dpa at temperatures between about 80 °C and 390 °C. Tensile tests were conducted at room and irradiation temperatures. The results demonstrate that the irradiation induced significant hardening and embrittlement in the specimens. The irradiation hardening and embrittlement effects show a trend of saturation at doses above about 10 dpa. Although the ductility was greatly reduced, all specimens broke with strong necking, which indicates a ductile fracture mode.     

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.     

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.     

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.     

Susceptibility to LME of 316L and T91 steels by LBE: Effect of strain rate

The effect of liquid lead-bismuth eutectic on 316L and T91 steels at 160 °C has been studied as a function of strain rate, using a centre cracked in tension specimen adapted for the study of crack propagation. Brittle fracture, characterized by elongated river cracks on all the fracture surfaces, indicates that T91 is sensitive to the embrittlement by LBE. This embrittlement effect is very pronounced at low deformation rate (∼10⁻⁵ mm s⁻¹). A ductile-brittle transition is observed in the high strain rate range investigated. In the transitory regime, there is a competition between the growth of dimples and brittle cracking induced by the liquid metal. Ductility recovery is complete at the highest investigated deformation rate. The mechanical properties of the 316L steel are not clearly affected by the presence of LBE, in spite of a modification in the plastic deformation mode which strongly affects fracture surfaces.     

WEBEXPIR: Windowless target electron beam experimental irradiation

The windowless target electron beam experimental irradiation (WEBEXPIR) program was set-up as part of the MYRRHA/XT-ADS R&D effort on the spallation target design to investigate the interaction of a proton beam with a liquid lead-bismuth eutectic (LBE) free surface. In particular, possible free surface distortion or shockwave effects in nominal conditions and during sudden beam on/off transient situations, as well as possible enhanced evaporation were assessed. An experiment was conceived at the IBA TT-1000 Rhodotron, where a 7 MeV electron beam was used to simulate the high power deposition at the MYRRHA/XT-ADS LBE free surface. The geometry and the LBE flow characteristics in the WEBEXPIR set-up were made as representative as possible of the actual situation in the MYRRHA/XT-ADS spallation target. Irradiation experiments were carried out at beam currents of up to 10 mA, corresponding to 40 times the nominal beam current necessary to reproduce the MYRRHA/XT-ADS conditions. Preliminary analyses show that the WEBEXPIR free surface flow was not disturbed by the interaction with the electron beam and that vacuum conditions stayed well within the design specifications.     

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.     

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.     

Proton irradiation emulation of PWR neutron damage microstructures in solution annealed 304 and cold-worked 316 stainless steels

Solution annealed (SA) 304 and cold-worked (CW) 316 austenitic stainless steels were pre-implanted with helium and were irradiated with protons in order to study the potential effects of helium, irradiation dose, and irradiation temperature on microstructural evolution, especially void swelling, with relevance to the behavior of austenitic core internals in pressurized water reactors (PWRs). These steels were irradiated with 1 MeV protons to doses between 1 and 10 dpa at 300 °C both with or without 15 appm helium pre-implanted at ∼100 °C. They were also irradiated at 340 °C, but only after 15 appm helium pre-implantation. Small heterogeneously distributed voids were observed in both alloys irradiated at 300 °C, but only after helium pre-implantation. The pre-implanted steels irradiated at 340 °C exhibited homogenous void formation, suggesting effects of both helium and irradiation temperature on void nucleation. Voids developed sooner in the SA304 alloy than CW316 alloy at 300 and 340 °C, consistent with the behavior observed at higher temperatures (>370 °C) for similar steels irradiated in the EBR-II fast reactor. The development of the Frank loop microstructure was similar in both alloys, and was only marginally affected by pre-implanted helium. Loop densities were insensitive to dose and irradiation temperature, and were decreased by helium; loop sizes increased with dose up to about 5.5 dpa and were not affected by the pre-implanted helium. Comparison with microstructures produced by neutron irradiation suggests that this method of helium pre-implantation and proton irradiation emulates neutron irradiation under PWR conditions.     

Polonium formation in Pb-55.5Bi under proton irradiation

Lead-bismuth eutectic (LBE) has been proposed both as spallation target and as coolant in a future accelerator driven system (ADS). The safety analyses require knowledge concerning the elements formed during proton irradiation, and their volatility. Discs of lead-bismuth eutectic (LBE) were irradiated with protons having 71 and 590 MeV energy resp. to analyse Po-isotopes formation. The generation of the isotopes Po 206 and 208 was clearly indicated. The ratio ²⁰⁶Po/²⁰⁸Po is dependent on the proton energy and as well on the beam intensity. In parallel to the analytical examinations calculations were carried out using the FLUKA Monte Carlo code to compare the analytical results with the calculations. The evaporation behaviour of irradiated LBE discs was examined as well whereby volatile Hg was found, but no Po evaporation was detected under the chosen conditions.     

Influence of Zn as a spallation product on the behaviour of martensitic steel T91 and austenitic steel 316L in liquid Pb-Bi

The liquid Pb-Bi alloy is proposed as material for the spallation target in hybrid systems. During the spallation process, several chemical elements are produced in the target which could generate specific liquid metal embrittlement phenomena. Among these species, zinc is known as an element which can promote LME (liquid metal embrittlement). Corrosion tests were carried out in liquid Pb-Bi in isothermal static conditions without and with 80 wppm of zinc at 150 °C, 350 °C and 600 °C up to 6000 h. No modification of the corrosion kinetics of T91 martensitic and 316L austenitic steels was observed for either unstressed or U-bend specimens with zinc in Pb-Bi. Moreover, no sign of embrittlement was observed for any of the samples with and without zinc.     

ADS散裂中子源材料不锈钢和钨的辐照效应(英文)

研究了80 MeV碳或85 MeV氟离子辐照在国产改进型316L不锈钢、普通不锈钢和钨中产生的辐照效应。实验结果表明,不锈钢的抗辐照性能比钨的好;它们中,国产改进型316L不锈钢具有最好的抗辐照性能。选用不锈钢做ADS散裂中子源的束窗等材料是较好的选择,采用国产改进型316L不锈钢是最佳的选择。     

Preliminary results of post-irradiation examinations on LiSoR-2 test section

Liquid-solid reaction under irradiation (LiSoR) experiments are aimed at understanding the effects of liquid lead-bismuth eutectic (LBE) corrosion and embrittlement under irradiation on structural materials, which is one of the key items of the materials R&D for the future accelerator-driven system (ADS). The LiSoR setup is basically a LBE loop with a test section irradiated with 72 MeV protons. The second irradiation was conducted for about 34 h and terminated after a leakage of LBE was detected. Post-irradiation examinations (PIE) are being performed on both the tube and tensile specimen in the test section. Optical microscopy, scanning electron microscopy, transmission electron microscopy and microhardness tests have been completed. The results show that a crack formed in the irradiation zone of the tube. In the material in the irradiation zones of both the tube and the tensile specimen dislocation cell structure is well developed, which indicates heavy deformation due to thermal fatigue. The crack should start at the inner surface and propagate to the outer surface. The fracture surfaces of the crack are dominated by a brittle cleavage fracture mode. However, on the surfaces of the tensile specimen, no microcracks are observed.     

Tensile properties of ferritic/martensitic steels irradiated in STIP-I

Specimens of ferritic/martensitic (FM) steels T91, F82H, Optimax-A and the electron beam weld (EBW) of F82H were irradiated in the Swiss spallation neutron source (SINQ) Target-3 in a temperature range of 90-370 °C to displacement doses between 3 and 12 dpa. Tensile tests were performed at room temperature and the irradiation temperatures. The tensile test results demonstrated that the irradiation hardening increased with dose up to about 10 dpa. Meanwhile, the uniform elongation decreased to less than 1%, while the total elongation remained greater than 5%, except for an F82H specimen of 9.8 dpa tested at room temperature, which failed in elastic deformation regime. At higher doses of 11-12 dpa, the ductility of some specimens recovered, which could be due to the annealing effect of a short period of high temperature excursion. The results do not show significant differences in tensile properties for the different FM steels in the present irradiation conditions.     

Corrosion behaviour of stainless steels in flowing LBE at low and high oxygen concentration

The corrosion behaviours of austenitic steel AISI 316L and martensitic steel T91 were investigated in flowing lead-bismuth eutectic (LBE) at 400 °C. The tests were performed in the LECOR and CHEOPE III loops, which stood for the low oxygen concentration and high oxygen concentration in LBE, respectively. The results obtained shows that steels were affected by dissolution at the condition of low oxygen concentration (C_[O2] = 10⁻⁸-10⁻¹⁰ wt%) and were oxidized at the condition of high oxygen concentration (C_[O2] = 10⁻⁵-10⁻⁶ wt%). The oxide layers detected are able to protect the steels from dissolution in LBE. Under the test condition adopted, the austenitic steel behaved more resistant to corrosion induced by LBE than the martensitic steel.     

Proton irradiation study of GFR candidate ceramics

This work investigated the microstructural response of SiC, ZrC and ZrN irradiated with 2.6 MeV protons at 800 °C to a fluence of 2.75 × 10¹⁹ protons/cm², corresponding to 0.71-1.8 displacement per atom (dpa), depending on the material. The change of lattice constant evaluated using HOLZ patterns is not observed. In comparison to Kr ion irradiation at 800 °C to 10 dpa from the previous studies, the proton irradiated ZrC and ZrN at 1.8 dpa show less irradiation damage to the lattice structure. The proton irradiated ZrC exhibits faulted loops which are not observed in the Kr ion irradiated sample. ZrN shows the least microstructural change from proton irradiation. The microstructure of 6H-SiC irradiated to 0.71 dpa consists of black dot defects at high density.     

Compatibility of martensitic/austenitic steel welds with liquid lead bismuth eutectic environment

The high-chromium ferritic/martensitic steel T91 and the austenitic stainless steel 316L are to be used in contact with liquid lead-bismuth eutectic (LBE), under high irradiation doses. Both tungsten inert gas (TIG) and electron beam (EB) T91/316L welds have been examined by means of metallography, scanning electron microscopy (SEM-EDX), Vickers hardness measurements and tensile testing both in inert gas and in LBE. Although the T91/316L TIG weld has very good mechanical properties when tested in air, its properties decline sharply when tested in LBE. This degradation in mechanical properties is attributed to the liquid metal embrittlement of the 309 buttering used in TIG welding of T91/316L welds. In contrast to mixed T91/316L TIG welding, the mixed T91/316L EB weld was performed without buttering. The mechanical behaviour of the T91/316L EB weld was very good in air after post weld heat treatment but deteriorated when tested in LBE.     

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.     

Tensile behaviour of 9Cr-1Mo tempered martensitic steels irradiated up to 20 dpa in a spallation environment

Tensile specimens of 9Cr-1Mo (EM10) and mod 9Cr-1Mo (T91) martensitic steels in the normalized and tempered metallurgical conditions were irradiated with high energy protons and neutrons up to 20 dpa at average temperatures up to about 360 °C. Tensile tests were carried out at room temperature and 250 °C and a few samples were tested at 350 °C. The fracture surfaces of selected specimens were characterized by Scanning Electron Microscopy (SEM). While all irradiated specimens displayed at room temperature considerable hardening and loss of ductility, those irradiated to doses above approximately 16 dpa exhibited a fully brittle behaviour and the SEM observations revealed significant amounts of intergranular fracture. Helium accumulation, up to about 0.18 at.% in the specimens irradiated to 20 dpa, is believed to be one of the main factors which triggered the brittle behaviour and intergranular fracture mode. One EM10 and one T91 specimen irradiated to 20 dpa were annealed at 700 °C for 1 h following irradiation and subsequently tensile tested. In both cases, a remarkable recovery of ductility and strain-hardening capacity was observed after annealing, while the strength remained significantly above that of the unirradiated material.