Monitoring bromide effect on radiolytic yields using in situ observations of uranyl oxide precipitation in the electron microscope
Abstract
During electron microscopy observations of uranium-bearing phases and solutions in a liquid cell, the electron beam induced radiolysis causes changes in the chemistry of the system. This could be useful for investigating accelerated alteration of UO2 and can be also used to monitor radiolytic effects. Low concentrations of bromide in aqueous solutions are known to reduce the generation rate of H2O2 during radiolysis and increase H2 production. We deduced the presence of radiolytic H2O2 by monitoring the formation of a uranyl peroxide solid from both solid UO2 and a solution of ammonium uranyl carbonate at neutral pH. Additionally, the effect of bromine on water radiolysis was investigated through chemical modelling and in situ electron microscopy. By measuring the contrast in the electron microscopy images it was possible to monitor H2O2 formation and diffusion from the irradiated zone in agreement with the models.
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1438092
- Alternate Identifier(s):
- OSTI ID: 1457763; OSTI ID: 1755152
- Report Number(s):
- PNNL-SA-128869
Journal ID: ISSN 2046-2069; RSCACL
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Published Article
- Journal Name:
- RSC Advances
- Additional Journal Information:
- Journal Name: RSC Advances Journal Volume: 8 Journal Issue: 33; Journal ID: ISSN 2046-2069
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Electron microscopy; in situ SEM; radiolysis; uranium
Citation Formats
Buck, Edgar C., Wittman, Richard S., Soderquist, Chuck. Z., and McNamara, Bruce K. Monitoring bromide effect on radiolytic yields using in situ observations of uranyl oxide precipitation in the electron microscope. United Kingdom: N. p., 2018.
Web. doi:10.1039/C8RA01706A.
Buck, Edgar C., Wittman, Richard S., Soderquist, Chuck. Z., & McNamara, Bruce K. Monitoring bromide effect on radiolytic yields using in situ observations of uranyl oxide precipitation in the electron microscope. United Kingdom. https://doi.org/10.1039/C8RA01706A
Buck, Edgar C., Wittman, Richard S., Soderquist, Chuck. Z., and McNamara, Bruce K. Mon .
"Monitoring bromide effect on radiolytic yields using in situ observations of uranyl oxide precipitation in the electron microscope". United Kingdom. https://doi.org/10.1039/C8RA01706A.
@article{osti_1438092,
title = {Monitoring bromide effect on radiolytic yields using in situ observations of uranyl oxide precipitation in the electron microscope},
author = {Buck, Edgar C. and Wittman, Richard S. and Soderquist, Chuck. Z. and McNamara, Bruce K.},
abstractNote = {During electron microscopy observations of uranium-bearing phases and solutions in a liquid cell, the electron beam induced radiolysis causes changes in the chemistry of the system. This could be useful for investigating accelerated alteration of UO2 and can be also used to monitor radiolytic effects. Low concentrations of bromide in aqueous solutions are known to reduce the generation rate of H2O2 during radiolysis and increase H2 production. We deduced the presence of radiolytic H2O2 by monitoring the formation of a uranyl peroxide solid from both solid UO2 and a solution of ammonium uranyl carbonate at neutral pH. Additionally, the effect of bromine on water radiolysis was investigated through chemical modelling and in situ electron microscopy. By measuring the contrast in the electron microscopy images it was possible to monitor H2O2 formation and diffusion from the irradiated zone in agreement with the models.},
doi = {10.1039/C8RA01706A},
journal = {RSC Advances},
number = 33,
volume = 8,
place = {United Kingdom},
year = {Mon Jan 01 00:00:00 EST 2018},
month = {Mon Jan 01 00:00:00 EST 2018}
}
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https://doi.org/10.1039/C8RA01706A
https://doi.org/10.1039/C8RA01706A
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Cited by: 6 works
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Figures / Tables:
Fig. 1: Method for determining the production of U-phase during irradiation.
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Figures / Tables found in this record:
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.