skip to main content

DOE PAGESDOE PAGES

Title: Monitoring bromide effect on radiolytic yields using in situ observations of uranyl oxide precipitation in the electron microscope

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 UO 2 and can be also used to monitor radiolytic effects. Low concentrations of bromide in aqueous solutions are known to reduce the generation rate of H 2O 2 during radiolysis and increase H 2 production. We deduced the presence of radiolytic H 2O 2 by monitoring the formation of a uranyl peroxide solid from both solid UO 2 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 H 2O 2 formation and diffusion from the irradiated zone in agreement with the models.
Authors:
ORCiD logo [1] ;  [1] ;  [1] ;  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-128869
Journal ID: ISSN 2046-2069; RSCACL
Grant/Contract Number:
AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 8; Journal Issue: 33; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Nuclear Energy (NE)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
OSTI Identifier:
1457763

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 States: N. p., 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 States. doi:10.1039/c8ra01706a.
Buck, Edgar C., Wittman, Richard S., Soderquist, Chuck. Z., and McNamara, Bruce K.. 2018. "Monitoring bromide effect on radiolytic yields using in situ observations of uranyl oxide precipitation in the electron microscope". United States. doi:10.1039/c8ra01706a. https://www.osti.gov/servlets/purl/1457763.
@article{osti_1457763,
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 States},
year = {2018},
month = {5}
}