Nucleation and growth of lead oxide particles in liquid lead-bismuth eutectic

文献情報

出版日 2017-10-05

DOI 10.1039/C7CP05068B

インパクトファクター 3.676

著者

Kris Rosseel, Jun Lim, Alessandro Marino, Geraldine Heynderickx, Alexander Aerts

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要旨

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.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.