Microscale Electrochemical Corrosion of Uranium Oxide Particles

Understanding the corrosion of spent nuclear fuel is important for the development of long-term storage solutions. However, the risk of radiation contamination presents challenges for experimental analysis. Adapted from the system for analysis at the liquid–vacuum interface (SALVI), we developed a m...

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Main Authors: Jiyoung Son, Shawn L. Riechers, Xiao-Ying Yu
Format: Article
Language:English
Published: MDPI AG 2023-09-01
Series:Micromachines
Subjects:
Online Access:https://www.mdpi.com/2072-666X/14/9/1727
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author Jiyoung Son
Shawn L. Riechers
Xiao-Ying Yu
author_facet Jiyoung Son
Shawn L. Riechers
Xiao-Ying Yu
author_sort Jiyoung Son
collection DOAJ
description Understanding the corrosion of spent nuclear fuel is important for the development of long-term storage solutions. However, the risk of radiation contamination presents challenges for experimental analysis. Adapted from the system for analysis at the liquid–vacuum interface (SALVI), we developed a miniaturized uranium oxide (UO<sub>2</sub>)-attached working electrode (WE) to reduce contamination risk. To protect UO<sub>2</sub> particles in a miniatured electrochemical cell, a thin layer of Nafion was formed on the surface. Atomic force microscopy (AFM) shows a dense layer of UO<sub>2</sub> particles and indicates their participation in electrochemical reactions. Particles remain intact on the electrode surface with slight redistribution. X-ray photoelectron spectroscopy (XPS) reveals a difference in the distribution of U(IV), U(V), and U(VI) between pristine and corroded UO<sub>2</sub> electrodes. The presence of U(V)/U(VI) on the corroded electrode surface demonstrates that electrochemically driven UO<sub>2</sub> oxidation can be studied using these cells. Our observations of U(V) in the micro-electrode due to the selective semi-permeability of Nafion suggest that interfacial water plays a key role, potentially simulating a water-lean scenario in fuel storage conditions. This novel approach offers analytical reproducibility, design flexibility, a small footprint, and a low irradiation dose, while separating the α-effect. This approach provides a valuable microscale electrochemical platform for spent fuel corrosion studies with minimal radiological materials and the potential for diverse configurations.
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spelling doaj.art-ad426c495bf04fd4a0219b5787d5ba172023-11-19T11:59:48ZengMDPI AGMicromachines2072-666X2023-09-01149172710.3390/mi14091727Microscale Electrochemical Corrosion of Uranium Oxide ParticlesJiyoung Son0Shawn L. Riechers1Xiao-Ying Yu2Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA 99354, USAEnergy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA 99354, USAOak Ridge National Laboratory, Materials Science and Technology Division, Oak Ridge, TN 37830, USAUnderstanding the corrosion of spent nuclear fuel is important for the development of long-term storage solutions. However, the risk of radiation contamination presents challenges for experimental analysis. Adapted from the system for analysis at the liquid–vacuum interface (SALVI), we developed a miniaturized uranium oxide (UO<sub>2</sub>)-attached working electrode (WE) to reduce contamination risk. To protect UO<sub>2</sub> particles in a miniatured electrochemical cell, a thin layer of Nafion was formed on the surface. Atomic force microscopy (AFM) shows a dense layer of UO<sub>2</sub> particles and indicates their participation in electrochemical reactions. Particles remain intact on the electrode surface with slight redistribution. X-ray photoelectron spectroscopy (XPS) reveals a difference in the distribution of U(IV), U(V), and U(VI) between pristine and corroded UO<sub>2</sub> electrodes. The presence of U(V)/U(VI) on the corroded electrode surface demonstrates that electrochemically driven UO<sub>2</sub> oxidation can be studied using these cells. Our observations of U(V) in the micro-electrode due to the selective semi-permeability of Nafion suggest that interfacial water plays a key role, potentially simulating a water-lean scenario in fuel storage conditions. This novel approach offers analytical reproducibility, design flexibility, a small footprint, and a low irradiation dose, while separating the α-effect. This approach provides a valuable microscale electrochemical platform for spent fuel corrosion studies with minimal radiological materials and the potential for diverse configurations.https://www.mdpi.com/2072-666X/14/9/1727uranium oxide (UO<sub>2</sub>)particle-attached electrodemicroscale electrochemical cellmultimodal characterizationNafion membranesystem for analysis at the liquid–vacuum interface (SALVI)
spellingShingle Jiyoung Son
Shawn L. Riechers
Xiao-Ying Yu
Microscale Electrochemical Corrosion of Uranium Oxide Particles
Micromachines
uranium oxide (UO<sub>2</sub>)
particle-attached electrode
microscale electrochemical cell
multimodal characterization
Nafion membrane
system for analysis at the liquid–vacuum interface (SALVI)
title Microscale Electrochemical Corrosion of Uranium Oxide Particles
title_full Microscale Electrochemical Corrosion of Uranium Oxide Particles
title_fullStr Microscale Electrochemical Corrosion of Uranium Oxide Particles
title_full_unstemmed Microscale Electrochemical Corrosion of Uranium Oxide Particles
title_short Microscale Electrochemical Corrosion of Uranium Oxide Particles
title_sort microscale electrochemical corrosion of uranium oxide particles
topic uranium oxide (UO<sub>2</sub>)
particle-attached electrode
microscale electrochemical cell
multimodal characterization
Nafion membrane
system for analysis at the liquid–vacuum interface (SALVI)
url https://www.mdpi.com/2072-666X/14/9/1727
work_keys_str_mv AT jiyoungson microscaleelectrochemicalcorrosionofuraniumoxideparticles
AT shawnlriechers microscaleelectrochemicalcorrosionofuraniumoxideparticles
AT xiaoyingyu microscaleelectrochemicalcorrosionofuraniumoxideparticles