Microscale Electrochemical Corrosion of Uranium Oxide Particles

Jiyoung Son; Shawn L. Riechers; Xiao Ying Yu

doi:10.3390/mi14091727

Microscale Electrochemical Corrosion of Uranium Oxide Particles

Jiyoung Son, Shawn L. Riechers, Xiao Ying Yu

Research output: Contribution to journal › Article › peer-review

Abstract

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 (UO₂)-attached working electrode (WE) to reduce contamination risk. To protect UO₂ 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 UO₂ 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 UO₂ electrodes. The presence of U(V)/U(VI) on the corroded electrode surface demonstrates that electrochemically driven UO₂ 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.

Original language	English
Article number	1727
Journal	Micromachines
Volume	14
Issue number	9
DOIs	https://doi.org/10.3390/mi14091727
State	Published - Sep 2023
Externally published	Yes

Funding

This research was funded by DOE Nuclear Energy Spent Fuel Waste Science Technology (SFWST) program. Part of the electrode surface property characterization was supported under the Direct Air Capture (DAC) Program, which was jointly supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Divisions of Chemical Sciences, Geosciences, and Biosciences (CSGB) and Materials Sciences and Engineering (MSE) under FWP 76830. Xiao-Ying Yu is grateful for the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL) for partial support of this work. Measurements of radiological specimens were performed at the Radiological Processing Laboratory (RPL) microscopy suite at the Pacific Northwest National Laboratory (PNNL). Radiological XPS was performed in the 331 Building at PNNL. The authors are grateful for technical assistance, comments, and suggestions on the XPS analysis from Nabajit Lahiri, Eugene Ilton, and Mark Engelhard. The authors are indebted to Jun Gao, Carolyne Burns, and Richard Daniel for their assistance in Raman spectroscopy and surface tension measurements. The authors also thank the administrative and technical support of Karrie Clark and Paul Martin for acquiring supplies and consumables. The authors thank Radiological Protection Professionals (RPTs) at PNNL for their administrative assistance in device radiation monitoring. ORNL is managed by UT-Battelle, LLC, for the U.S. Department of Energy (DOE) under contract number DE-AC05-00OR22725. PNNL is operated for the U.S. DOE by Battelle Memorial Institute under Contract No. DE-AC05-76RL01830. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. DOE. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ) accessed on 5 June 2023 upon publication.

Funders	Funder number
DOE Nuclear Energy Spent Fuel Waste Science Technology
Laboratory Directed Research
SFWST
U.S. Department of Energy	DE-AC05-00OR22725
Battelle	DE-AC05-76RL01830
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Division of Materials Sciences and Engineering	FWP 76830
Chemical Sciences, Geosciences, and Biosciences Division

Keywords

microscale electrochemical cell
multimodal characterization
Nafion membrane
particle-attached electrode
system for analysis at the liquid–vacuum interface (SALVI)
uranium oxide (UO)

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.3390/mi14091727

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abstract = "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 (UO2)-attached working electrode (WE) to reduce contamination risk. To protect UO2 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 UO2 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 UO2 electrodes. The presence of U(V)/U(VI) on the corroded electrode surface demonstrates that electrochemically driven UO2 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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N2 - 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 (UO2)-attached working electrode (WE) to reduce contamination risk. To protect UO2 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 UO2 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 UO2 electrodes. The presence of U(V)/U(VI) on the corroded electrode surface demonstrates that electrochemically driven UO2 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.

AB - 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 (UO2)-attached working electrode (WE) to reduce contamination risk. To protect UO2 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 UO2 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 UO2 electrodes. The presence of U(V)/U(VI) on the corroded electrode surface demonstrates that electrochemically driven UO2 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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Microscale Electrochemical Corrosion of Uranium Oxide Particles

Abstract

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Keywords

UN SDGs

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