Wavelength dependent neutron transmission and radiography investigations of the high temperature behaviour of materials applied in nuclear fuel and control rod claddings

Neutron radiography was used for the investigation of the nuclear fuel and control rod cladding behaviour during steam oxidation under severe nuclear accident conditions. In order to verify the hypothesis that the unexpectedly high neutron cross-section found after oxidation of Zircaloy-4 in wet air containing 10% steam is caused by a strong hydrogen uptake, the wavelength dependence of the total macroscopic neutron cross-section of the specimens was measured. The characteristic dependence for hydrogen was not found, which is a proof that hydrogen is not absorbed significantly. The data agree mostly with the behaviour expected for β-Zr.Examinations of control rod simulators annealed until the failure in single-rod tests were performed. In order to separate the effect of the neutron absorber and control rod structure materials, radiographs taken with different neutron spectra were combined. This procedure clearly showed that the local melting resulting from the eutectic reaction between the stainless steel control rod cladding and the Zircaloy-4 guide tube is the reason for the failure.     

Study of hydrogen effusion in austenitic stainless steel by time-resolved in-situ measurements using neutron radiography

The purpose of the present study was to show the feasibility of measuring hydrogen effusion in austenitic stainless steel (1.4301) using neutron radiography at the facility ANTARES of the research reactor FRM II of the Technische Universität München. This method is appropriate to measure in-situ hydrogen effusion for hydrogen concentrations as small as 20 ppm_H. Experiments were carried out in the temperature range from room temperature up to 533 K. The measurement principle is based on the parallel comparison of electrochemically hydrogen charged specimen with hydrogen-free reference specimen at the same temperature. This allows the determination of the hydrogen concentration in the specimens as a function of time and temperature. Separate hot carrier gas extraction experiments using the same temperature-time profiles as the radiography experiments have been used to calibrate the grey values of the neutron transmission images into hydrogen concentrations. It can be stated that the hydrogen effusion correlates with the specimen temperature.     

Measurements of water distribution in through-plane direction of PEFC by using neutron radiography

Fuel gas (hydrogen gas) and oxidant gas (air) are supplied to a polymer electrolyte fuel cell (PEFC). Protons pass through the electrolyte membrane, and combine with oxygen to form water in the cathode reaction site. The generated water must be supplied appropriately to the membrane for proton conduction. On the other hand, the generated water may affect the fuel cell performances because of the blocking of oxygen from reaching the cathode reaction site. Therefore, water management in the PEFC is important, and water distribution during the operation in the through-plane direction has been of wide concern. In order to obtain the water distributions in a membrane electrode assembly (MEA) and a gas diffusion layer (GDL), a borescope system was newly employed using neutron radiography. The system could obtain the water distribution in the MEA and the GDL, and pixel size of 6.5 μm was achieved. Furthermore, the system was applied for a tilted converter system. The pixel of 1.0 μm at an angle of 81° was achieved, and improvement of the spatial resolution was confirmed.     

Dehydration of moulding sand in simulated casting process examined with neutron radiography

Natural bentonites are an important material in the casting industry. Smectites as the main component of bentonites plasticize and stabilise sand moulds. Pore water as well as interlayer water within the smectites are lost as a function of time, location and temperature. Although rehydration of the smectites should be a reversible process, the industrially dehydrated smectites lose their capability to reabsorb water. This limits the number of possible process cycles of the mould material. A full understanding of the dehydration process would help to optimise the amount of fresh material to be added and thus save resources. A simulated metal casting was investigated with neutron radiography at the ANTARES neutron imaging facility of the FRM II reactor of Technische Universität München, Germany.     

实时中子照相系统图像斑状噪声迭代滤波算法

根据实时中子辐照图像“斑状”噪声的成因和特点,提出一种有效的迭代滤波算法。设计十字形噪声检测窗口,通过计算邻域一致性测度(NHM),将像素分为噪声和信号。对噪声进行迭代滤波,而对信号则不做任何处理。滤波是一个中值计算过程,同时窗宽可自适应调整。这种方案不仅避免了噪声在邻域的传播,且有较高的计算效率。实验结果表明,对于峰值信噪比(PSNR)为24.51dB的噪声污染图像,3×3中值滤波后PSNR只有26.81dB,而本文算法能将其提高到31.54dB,同时图像的视觉效果更好。     

Development of neutron radiography facility for boiling two-phase flow experiment in Kyoto University Research Reactor

To visualize boiling two-phase flow at high heat flux by using neutron radiography, a new neutron radiography facility was developed in the B-4 beam hole of KUR. The B-4 beam hole is equipped with a supermirror neutron guide tube with a characteristic wavelength of 1.2 Å, whose geometrical parameters of the guide tube are: 11.7 m total length and 10 mm wide ×74 mm high beam cross-section. The total neutron flux obtained from the KUR supermirror guide tube is about 5×10⁷ n/cm² s with a nominal thermal output of 5 MW of KUR, which is about 100 times what is obtainable with the conventional KUR neutron radiography facility (E-2 beam hole). In this study a new imaging device, an electric power supply (1200 A, 20 V), and a thermal hydraulic loop were installed. The neutron source, the beam tube, and the radiography rooms are described in detail and the preliminary images obtained at the developed facility are shown.     

The effects of neutron radiation on nickel-based alloys

The effects of neutron radiation on nickel-based alloys in thermal reactors are defying predictions that were made based upon accelerated testing in fast reactors. As nickel-based alloy components face significant doses in aging thermal reactors and their role in Gen-IV reactor designs becomes prominent, the literature on the effects of radiation on such alloys must be reviewed to enable better structural integrity assessments for relevant components and optimise alloys with respect to irradiation embrittlement resistance. This paper reviews the available data on the effects of radiation, notably neutron radiation, on nickel-based alloys and discusses the possible mitigation strategies and design opportunities for radiation embrittlement-resistant alloys based on recent developments in alloy computational design.

This review was submitted as part of the 2016 Materials Literature Review Prize of the Institute of Materials, Minerals and Mining run by the Editorial Board of MST. Sponsorship of the prize by TWI Ltd is gratefully acknowledged.     

Effects of catalytic surface layer on Zr-based alloy getters for hydrogen absorption

Hydrogen sorption characteristics of Zr-based alloy getters fabricated in the forms of bulk were investigated. Non-evaporable getters (NEGs) have been widely used in vacuum devices, but thermal activation process at high temperature and high vacuum environment is inevitably required for efficient sorption rate. In order to solve this problem and improve sorption kinetics, we developed and characterized Ni-coated NEGs. Ni-coated NEGs show good gettering performance and fast sorption kinetics without any activation process, compared to conventional Zr-based NEGs. It is mainly caused by the catalytic effect of surface Ni layer. Surface Ni plays an important role as a catalyst that enables hydrogen to dissociate on surface more easily and also as a protection layer against oxidation. Consequently, Ni-coated NEGs can be easily applicable to vacuum devices because those need not go through the activation process and show fast hydrogen sorption kinetics.     

Behaviour of hydrogen impurity in aluminium alloys during anodizing

The present study examines the behaviour of hydrogen impurity in an Al-6.5 at.% W alloy during anodizing, using elastic recoil detection and nuclear reaction analyses. Increased concentrations of hydrogen are found near the alloy/anodic film interface, amounting to ∼2×10¹⁵ H atoms cm⁻² for the particular alloy, containing 0.1-0.3 at.% hydrogen in the bulk regions, and conditions of anodizing. The enrichment arises from hydrogen in the alloy (i) diffusing to the interface, which acts as a trap, or (ii) accumulating at the interface, due to the growth of the anodic film, or a combination of both processes. Diffusion is consistent with the known mobility of hydrogen in aluminium near ambient temperature. Further, accumulation, and subsequent oxidation, of hydrogen are expected based on the general behaviour of alloying elements in anodized aluminium. The anodic films contained ∼0.1-0.3 at.% hydrogen, originating from either the electrolyte or the alloy.     

Scatter rejection in quantitative thermal and cold neutron imaging

The accuracy of quantitative neutron transmission radiography can be substantially decreased if highly scattering materials, such as water or plastics, exist in the sample. There are currently two main solutions to this problem: either performing experiments at a large distance between the detector and the sample or employ some numerical correction techniques. In the former case, the spatial resolution is substantially reduced by the limited beam divergence, while the latter correction requires a priori information about the sample and is limited to distances of above ∼2 cm. We demonstrate the feasibility of another technique, namely the possibility to remove the scattered neutron component from the transmitted neutron beam by a very compact polycapillary collimator. These ∼1 mm thick devices can be placed between the sample and the detector and remove most of the neutrons scattered at angles larger than the acceptance angle of the collimator (typically 1°). No image distortions above ∼10 μm scales are introduced by these collimators. The neutron transmission of highly scattering samples (water and plexiglass) is measured in our experiments with and without scatter rejection. In the latter case, the accuracy of measured transmission coefficient was substantially improved by our collimators.     

高强韧锆合金的发展与应用

锆及其合金具有较好的尺寸稳定性、抗辐照和耐腐蚀等性能,因此在航空航天、航海、核反应堆和生物医用等领域具有重要的应用前景.而纯锆及应用较为广泛的锆合金的抗拉强度较低,提升锆及其合金的力学性能成为其能成功应用于结构件的关键环节.本文简要概述了锆及其合金在核工业、化工、医疗及航空航海等领域的发展现状.此外,本文还着重介绍了新型高强韧锆合金的设计与制备,获取了可在空间探测、深海探测以及高速铁路等特殊领域中使用的锆系合金的最佳成分,并详细阐述了新型高强韧锆合金的强化机理及其在核电、化工及航空领域中的应用.     

Application of neutron radiography in observing and quantifying the time-dependent moisture distributions in multi-cracked cement-based composites

Significant tensile strain capacity of SHCC under tensile stress can be reached by multi-crack formation, while the cracks remain bridged by fibres. Ductility of SHCC is due to this multi-crack formation. Cracks are preferential pathways for ingress of water and salt solutions into the material. In this contribution neutron radiography has been successfully applied to visualize the process of water penetration into cracked SHCC and to quantify the corresponding time-dependent moisture distributions in cracked SHCC. Results indicate that in uncracked SHCC, less water can be found. Once cracked, however, both the amount of water and the penetration depth increased with increasing of crack density and the wider crack pattern when higher tensile strain was applied. Even at comparatively modest imposed strain when micro-cracks were formed, water penetrated into the specimens along the cracks of 30 μm–50 μm immediately and then water migrated further into the surrounding matrix from water filled cracks. Water then moved into the matrix adjacent to the cracks which was mechanically damaged by direct tension. Therefore, if durability of SHCC is an issue for application, a maximum strain may not be exceeded. In order to prevent penetration of water or salt solutions into cracked SHCC, two approaches were used. Integral water repellent SHCC was prepared by adding silane emulsion to the fresh mortar. Compared with neat SHCC, the integral water repellent SHCC with multi-cracks absorbed much less water after imposed to the same tensile strain. Notice that there was still a small amount of moisture that could enter the matrix of integral water repellent SHCC via cracks when the tensile strain was over 1.5% in this study. As an alternative method, surface impregnation with silane gel was a more promising approach to protect cracked SHCC from water or salt solution penetration into the material when multi-cracks formed.     

The review and prospect of neutron radiography in China

Neutron radiography is one of radiography ray non-destructive testing. It is a valuable complementary of X and γ rays radiography. This paper briefly describes the history of neutron radiography in China, and introduces the status of neutron radiography facilities and their development in China.     

Neutron radiography observations of inner wet region in drying of quartz sand cylinder

The drying process of wet quartz sand cylinder was studied with neutron radiography as well as with sample temperature and mass measurements. The constant rate and falling rate periods of the process were clearly identified. During the advanced phase of drying, an inner wet region in the sample center was revealed in the neutron radiographs. The emergence of the inner wet region resulted in marked rise in the standard deviation of the brightness of pixels constituting the sample image. The theoretical analysis of the brightness variations was performed in terms of neutron absorption in dry material matrix and water occupying some of the space between sand grains as well as scattering of neutrons on water. It was found that the inner wet region shrinks in radial direction with time while the apparent water content within it remains constant. The different periods of drying have been attributed to capillary transport at the beginning and vapor flow at advanced stages of the process.     

Visualization of hydrogen diffusion in steels by high sensitivity hydrogen microprint technique

Hydrogen diffusion in steels was examined by both a high sensitivity hydrogen microprint technique (HMT) and an electrochemical hydrogen permeation method. The main diffusion path in an extremely low carbon steel was lattice within grains; grain boundaries were not accelerated diffusion paths. In the case of a hypo-eutectoid steel, hydrogen diffused through proeutectoid ferrite and ferrite in pearlite under steady-state of hydrogen diffusion. The diffusion paths, however, were carbide/ferrite interfaces when hydrogen charging was interrupted before achievement of the steady state. This is probably ascribable to the reversible trapping effect of the interface. The detection efficiency of the high sensitivity HMT was 75% for the low carbon steel and 40% for the hypo-eutectoid steel.     

Evaluation of water distribution in a small operating fuel cell using neutron color image intensifier

Neutron radiography is one of the useful tools for visualizing water behavior in operating fuel cells. In order to observe the detailed information about the water distribution in membrane electrode assembly (MEA) and gas diffusion layer (GDL) in fuel cells, a high performance neutron imaging system is required. A neutron color image intensifier (NCII) is a high spatial resolution and high sensitivity neutron image detector. We have developed an imaging system using an NCII for visualizing the behavior of water in fuel cells. The pixel size of the imaging system is around 4.7 μm in the small view field. By using this system, water distribution of a small sized fuel cell was observed continuously every 20 s at the Thermal Neutron Radiography Facility (TNRF). In the results, the water area appears from the GDL and MEA regions, and expanded to the cathode side channel with time. However, the voltage was gradually reduced with time, and steeply dropped. It is considered that the reduction and the drop of voltage were caused by a blockage of gas flow due to accumulation of water in the GDL and the gas flow channel in the cathode side.     

Visualization of hydrogen diffusion in steels by high sensitivity hydrogen microprint technique

Hydrogen diffusion in steels was examined by both a high sensitivity hydrogen microprint technique (HMT) and an electrochemical hydrogen permeation method. The main diffusion path in an extremely low carbon steel was lattice within grains; grain boundaries were not accelerated diffusion paths. In the case of a hypo-eutectoid steel, hydrogen diffused through proeutectoid ferrite and ferrite in pearlite under steady-state of hydrogen diffusion. The diffusion paths, however, were carbide/ferrite interfaces when hydrogen charging was interrupted before achievement of the steady state. This is probably ascribable to the reversible trapping effect of the interface. The detection efficiency of the high sensitivity HMT was 75% for the low carbon steel and 40% for the hypo-eutectoid steel.     

Determination of the parahydrogen fraction in a liquid hydrogen target using energy-dependent slow neutron transmission

The NPDGamma collaboration is performing a measurement of the very small parity-violating asymmetry in the angular distribution of the 2.2 MeV γ-rays from the capture of polarized cold neutrons on protons (A_γ). The estimated size of A_γ is 5×10⁻⁸, and the measured asymmetry is proportional to the neutron polarization upon capture. Since the interaction of polarized neutrons with one of the two hydrogen molecular states (orthohydrogen) can lead to neutron spin-flip scattering, it is essential that the hydrogen in the target is mostly in the molecular state that will not depolarize the neutrons (≥99.8% parahydrogen). For that purpose, in the first stage of the NPDGamma experiment at the Los Alamos Neutron Science Center (LANSCE), we operated a 16-l liquid hydrogen target, which was filled in two different occasions. The parahydrogen fraction in the target was accurately determined in situ by relative neutron transmission measurements. The result of these measurements indicate that the fraction of parahydrogen in equilibrium was 0.9998±0.0002 in the first data taking run and 0.9956±0.0002 in the second. We describe the parahydrogen monitor system, relevant aspects of the hydrogen target, and the procedure to determine the fraction of parahydrogen in the target. Also assuming thermal equilibrium of the target, we extract the scattering cross-section for neutrons on parahydrogen.     

In-situ study on hydrogen bubble evolution in the liquid Al/solid Ni interconnection by synchrotron radiation X-ray radiography

Synchrotron X-ray radiography was used to carry out an in-situ observation of the hydrogen bubble evolution in the liquid Al/solid Ni interconnection. The individual bubble mainly grows in a stochastic way during heating. The size distribution for groups of bubbles follows a Gaussian distribution in the early stage and Lifshitz-Slyozov-Wagner (LSW) diffusion controlled distribution in the final stage. The intermetallic compounds (IMCs) first form during solidification, following by the hydrogen bubbles. The bubbles between two adjacent Al₃Ni grains grow unidirectionally along the liquid channel, with the bottom being impeded by the Al₃Ni phase and the radius of the growth front being smaller. For the bubbles at triple junctions, they grow along the liquid channel and the crack with morphology transition.     

Evaluations of the new LiF-scintillator and optional brightness enhancement films for neutron imaging

Japan Atomic Energy Agency has developed the neutron scintillator jointly with Chichibu Fuji Co., Ltd. In this study, we evaluated the new ZnS(Ag):Al/⁶Li scintillator developed for neutron imaging. It was confirmed that the brightness increased by about double while maintaining equal performance for the spatial resolution as compared with a conventional scintillator. High frame-rate imaging using a high-speed video camera system and this new scintillator made it possible to image beyond 10 000 frames per second while still having enough brightness. This technique allowed us to obtain a high-frame-rate visualization of oil flow in a running car engine. Furthermore, we devised a technique to increase the light intensity of reception for a camera by adding brightness enhancement films on the output surface of the scintillator. It was confirmed that the spatial resolution degraded more than double, but the brightness increased by about three times.