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Production and Characterization of Monodisperse Plutonium, Uranium, and Mixed Uranium–Plutonium Particles for Nuclear Safeguard Applications

Ranebo, Ylva LU ; Niagolova, Nedialka; Erdmann, Nicole; Tamborini, Gabriele and Betti, Maria (2010) In Analytical Chemistry 82(10). p.4055-4062
Abstract
In Safeguards work under the Non-Proliferation Treaty, the isotopic analysis of

uranium and plutonium micro particles has strengthened the means for detecting

undeclared nuclear activities. In order to assure accuracy and precision in the

analytical methodologies used, the instrumental techniques need to be calibrated.

The objective of this study was to produce and characterize particles consisting of

U, Pu and mixed U–Pu, suitable for such reliability verifications. A TSI vibrating

orifice aerosol generator in connection with a furnace system was used to produce

micrometer sized, monodispersed particles from reference U and Pu materials in

solutions. The particle... (More)
In Safeguards work under the Non-Proliferation Treaty, the isotopic analysis of

uranium and plutonium micro particles has strengthened the means for detecting

undeclared nuclear activities. In order to assure accuracy and precision in the

analytical methodologies used, the instrumental techniques need to be calibrated.

The objective of this study was to produce and characterize particles consisting of

U, Pu and mixed U–Pu, suitable for such reliability verifications. A TSI vibrating

orifice aerosol generator in connection with a furnace system was used to produce

micrometer sized, monodispersed particles from reference U and Pu materials in

solutions. The particle masses (in the range of 3-6 pg between batches) and sizes

(~1.5 μm) were controlled by the experimental conditions and the parameters for

the aerosol generator. Size distributions were obtained from scanning electron

microscopy, and energy-dispersive X-ray analysis confirmed that the particle

composition agreed with the starting material used. A secondary ion mass

spectrometer (SIMS) was used to characterize the isotopic composition of the

particles. Isobaric and polyatomic interference in the SIMS spectra was identified.

In order to obtain accurate estimates of the interference, a batch of Pu particles

were produced of mainly 242Pu. These were used for SIMS analysis to characterize

the behavior of Pu hydride and to determine the SIMS useful yields of U and Pu.

It was found that Pu had a higher propensity to form the hydride than U. Useful

yields were determined at a mass resolution of 450 for U–Pu particles: (1.71 ±

0.15) % for Pu and (0.72 ± 0.06) % for U, and for Pu particles: (1.65 ± 0.14) %

for Pu. This gave a relative sensitivity factor between U and Pu of 2.4 ± 0.2. (Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
vibrating orifice aerosol generator, plutonium oxide particles, uranium oxide particles, secondary ion mass spectrometry, scanning electron microscopy, nuclear safeguards
in
Analytical Chemistry
volume
82
issue
10
pages
4055 - 4062
publisher
The American Chemical Society
external identifiers
  • wos:000277531500014
  • scopus:77952507171
ISSN
1520-6882
DOI
10.1021/ac9029295
language
English
LU publication?
yes
id
50556d56-1d58-4dca-881a-e17ad53b6e37 (old id 1501594)
date added to LUP
2010-06-21 10:11:51
date last changed
2018-05-29 10:09:32
@article{50556d56-1d58-4dca-881a-e17ad53b6e37,
  abstract     = {In Safeguards work under the Non-Proliferation Treaty, the isotopic analysis of<br/><br>
uranium and plutonium micro particles has strengthened the means for detecting<br/><br>
undeclared nuclear activities. In order to assure accuracy and precision in the<br/><br>
analytical methodologies used, the instrumental techniques need to be calibrated.<br/><br>
The objective of this study was to produce and characterize particles consisting of<br/><br>
U, Pu and mixed U–Pu, suitable for such reliability verifications. A TSI vibrating<br/><br>
orifice aerosol generator in connection with a furnace system was used to produce<br/><br>
micrometer sized, monodispersed particles from reference U and Pu materials in<br/><br>
solutions. The particle masses (in the range of 3-6 pg between batches) and sizes<br/><br>
(~1.5 μm) were controlled by the experimental conditions and the parameters for<br/><br>
the aerosol generator. Size distributions were obtained from scanning electron<br/><br>
microscopy, and energy-dispersive X-ray analysis confirmed that the particle<br/><br>
composition agreed with the starting material used. A secondary ion mass<br/><br>
spectrometer (SIMS) was used to characterize the isotopic composition of the<br/><br>
particles. Isobaric and polyatomic interference in the SIMS spectra was identified.<br/><br>
In order to obtain accurate estimates of the interference, a batch of Pu particles<br/><br>
were produced of mainly 242Pu. These were used for SIMS analysis to characterize<br/><br>
the behavior of Pu hydride and to determine the SIMS useful yields of U and Pu.<br/><br>
It was found that Pu had a higher propensity to form the hydride than U. Useful<br/><br>
yields were determined at a mass resolution of 450 for U–Pu particles: (1.71 ±<br/><br>
0.15) % for Pu and (0.72 ± 0.06) % for U, and for Pu particles: (1.65 ± 0.14) %<br/><br>
for Pu. This gave a relative sensitivity factor between U and Pu of 2.4 ± 0.2.},
  author       = {Ranebo, Ylva and Niagolova, Nedialka and Erdmann, Nicole and Tamborini, Gabriele and Betti, Maria},
  issn         = {1520-6882},
  keyword      = {vibrating orifice aerosol
generator,plutonium oxide particles,uranium oxide particles,secondary ion mass
spectrometry,scanning electron microscopy,nuclear safeguards},
  language     = {eng},
  number       = {10},
  pages        = {4055--4062},
  publisher    = {The American Chemical Society},
  series       = {Analytical Chemistry},
  title        = {Production and Characterization of Monodisperse Plutonium, Uranium, and Mixed Uranium–Plutonium Particles for Nuclear Safeguard Applications},
  url          = {http://dx.doi.org/10.1021/ac9029295},
  volume       = {82},
  year         = {2010},
}