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Title: 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.

Authors:
ORCiD logo [1];  [1];  [1];  [1]
  1. Pacific Northwest National Laboratory, Richland, USA
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1438092
Alternate Identifier(s):
OSTI ID: 1457763
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 (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

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. doi: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. doi: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 = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/C8RA01706A

Figures / Tables:

Fig. 1 Fig. 1: Method for determining the production of U-phase during irradiation.

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