Abstract:Iron released by steel corrosion was found to be a key impurity in reactions with dissolved oxygen in liquid lead-bismuth eutectic alloys. The iron-oxygen-magnetite equilibrium was characterized, allowing the quantification of phenomena that are important for long-term operation of lead-alloy based installations such as corrosion rate control and management of precipitates.
“…Heterogeneous nucleation in LBE is considered possible because of the relatively large number of impurity particles present in the LBE under the conditions tested. Solid oxides, such as magnetite, 24 can be present in LBE in contact with stainless steel surfaces. The results presented here show comparable values of oversaturation independent of the LBE residence time in the experimental setups, suggesting the absence of dependency on corrosion product impurity content.…”
a Liquid lead-bismuth eutectic (LBE) is an important candidate to become the primary coolant of future, generation IV, nuclear fast reactors and Accelerator Driven System (ADS) concepts. One of the main challenges with the use of LBE as a coolant is to avoid its oxidation which results in solid lead oxide (PbO) precipitation. The chemical equilibria governing PbO formation are well understood. However, insufficient kinetic information is currently available for the development of LBE-based nuclear technology. Here, we report the results of experiments in which the nucleation, growth and dissolution of PbO in LBE during temperature cycling are measured by monitoring dissolved oxygen using potentiometric oxygen sensors. The metastable region, above which PbO nucleation can occur, has been determined under conditions relevant for the operation of LBE cooled nuclear systems and was found to be independent of setup geometry and thus thought to be widely applicable. A kinetic model to describe formation and dissolution of PbO particles in LBE is proposed, based on Classical Nucleation Theory (CNT) combined with mass transfer limited growth and dissolution. This model can accurately predict the experimentally observed changes in oxygen concentration due to nucleation, growth and dissolution of PbO, using the effective interfacial energy of a PbO nucleus in LBE as a fitting parameter.The results are invaluable to evaluate the consequences of oxygen ingress in LBE cooled nuclear systems under normal operating and accidental conditions and form the basis for the development of cold trap technology to avoid PbO formation in the primary reactor circuit.
“…Heterogeneous nucleation in LBE is considered possible because of the relatively large number of impurity particles present in the LBE under the conditions tested. Solid oxides, such as magnetite, 24 can be present in LBE in contact with stainless steel surfaces. The results presented here show comparable values of oversaturation independent of the LBE residence time in the experimental setups, suggesting the absence of dependency on corrosion product impurity content.…”
a Liquid lead-bismuth eutectic (LBE) is an important candidate to become the primary coolant of future, generation IV, nuclear fast reactors and Accelerator Driven System (ADS) concepts. One of the main challenges with the use of LBE as a coolant is to avoid its oxidation which results in solid lead oxide (PbO) precipitation. The chemical equilibria governing PbO formation are well understood. However, insufficient kinetic information is currently available for the development of LBE-based nuclear technology. Here, we report the results of experiments in which the nucleation, growth and dissolution of PbO in LBE during temperature cycling are measured by monitoring dissolved oxygen using potentiometric oxygen sensors. The metastable region, above which PbO nucleation can occur, has been determined under conditions relevant for the operation of LBE cooled nuclear systems and was found to be independent of setup geometry and thus thought to be widely applicable. A kinetic model to describe formation and dissolution of PbO particles in LBE is proposed, based on Classical Nucleation Theory (CNT) combined with mass transfer limited growth and dissolution. This model can accurately predict the experimentally observed changes in oxygen concentration due to nucleation, growth and dissolution of PbO, using the effective interfacial energy of a PbO nucleus in LBE as a fitting parameter.The results are invaluable to evaluate the consequences of oxygen ingress in LBE cooled nuclear systems under normal operating and accidental conditions and form the basis for the development of cold trap technology to avoid PbO formation in the primary reactor circuit.
“…where solids and dissolved species are indicated by (s) and (lbe), respectively. This reaction was also found to have a strong impact on the local oxygen concentration and precipitate formation in larger LBE installations such as the CRAFT corrosion loop [15]. Large differences of the oxygen concentration between the hot leg, where the oxygen control point was located, and the cold leg were observed under certain conditions.…”
Section: Impurity Chemistry and Managementmentioning
confidence: 87%
“…One of the abundant corrosion products expected to be released in the LBE of MYRRHA is iron. The reaction between dissolved iron, and dissolved oxygen in liquid LBE has been characterized [15]. It was found that many experimental observations, such as the change of dissolved oxygen concentration during temperature changes in a system with constant composition, can be described by the simple equilibrium:…”
Section: Impurity Chemistry and Managementmentioning
confidence: 99%
“…The trend in the cold zone starts deviating from that in the hot zone after about 65 h due to magnetite precipitation, as indicated by the arrows. The inset shows the evolution of hot and cold zone oxygen concentrations in the magnetite solubility product diagram[15].…”
Compatibility with structural materials and activation are major challenges of the use of heavy liquid metal (HLM) spallation targets and coolants such as lead-bismuth eutectic (LBE). Steel exposed to HLM is prone to corrosion which results in the release of steel elements in the HLM coolant. A commonly accepted strategy to reduce corrosion rates is to maintain a sufficiently elevated dissolved oxygen concentration in order to stabilize a protective oxide layer on the steel surface in contact with HLM. We present a brief overview of the oxygen sensing and control technology for LBE, developed in the frame of the MYRRHA accelerator driven system (ADS) demonstrate its performance on a large scale in the MEXICO chemistry loop (Mass Exchanger In Continuous Operation). MYRRHA stands for Multipurpose hYbrid Research Reactor for High-tech Applications accelerator driven system and is currently under development at the Belgian Nuclear Research Centre, and will operate between 200 °C and 400 °C with a target oxygen concentration level of 10-7 wt-%. Numerical simulations allowed mapping of the local oxygen concentration in MYRRHA, enabling identification of the regions in the core which could be prone to corrosion. On the other hand, oxygen concentrations must be sufficiently low to avoid formation of solid lead oxide (PbO) in the primary circuit. When designing a nuclear system such as an ADS, one must take into account accidents that may lead to increase of the oxygen concentration in the LBE and assess the probability for PbO formation and its consequences. In this context, we have studied the formation of lead oxide from oxygen-oversaturated LBE and determined the metastable limit for PbO nucleation. Corrosion products that are released in the LBE will interact with dissolved oxygen in LBE to form corrosion product oxides. These interactions influence the concentration of both dissolved oxygen and dissolved corrosion products. This in turn can cause changes in the corrosion process itself by altering the driving force for steel element dissolution or protective oxide layer decomposition. Experimental results will be presented which provide evidence for the precipitation and dissolution of oxides of iron impurities in LBE. Numerical simulations based on computational fluid dynamics (CFD) and chemical equilibrium complement experiments in understanding the interactions between coolant chemistry and reactor thermal-hydraulics. A similar approach was adopted for simulating the chemistry of spallation and other radioactive impurities in the primary LBE of MYRRHA. Simulations allow the prediction of released fraction, vapor composition and precipitation/dissolution phenomena in the LBE, as function of the oxygen concentration in the LBE and of the oxygen and humidity content of the cover gas in contact with the LBE. Simulations of the chemical behavior of several critical
“…In 2016, SCK-CEN has investigated the saturation concentration of Fe in LBE of different oxygen concentration [13] and the relation is given by Eq. (3)…”
For better understanding the corrosion and corrosion products behavior in the primary circuit of lead-bismuth eutectic (LBE) coolant reactor, the concentration distribution of soluble impurities and the transport of solid particles are investigated through finite-element method. An axisymmetric model of the primary circuit of LBE reactor was constructed to accelerate the calculation the thermal hydraulic filed of circuit. The saturation concentration of solute Fe, Cr and Ni in LBE coolant are identified through the equilibrium of their oxides and PbO. And the very different saturation concentrations of Fe/Cr/Ni in LBE will lead to significant element selective corrosion. The migration of solid oxides particles in the primary circuit is also investigated by the Euler-Lagrange tracing model. The simulation shows that driving force for the movement of particles >100 μm is buoyancy, which lets particles float on a free surface, while particles <10 μm tend to suspend in coolant. However, the behavior of particles also depends on the formation position, the particles formed above the core have the high possibility of re-entering in the core.
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