A new highly enriched 233U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

Richard M. Essex; Ross W. Williams; Kayron T. Rogers; Cole R. Hexel; Tashi Parsons-Davis; Kerri C. Treinen

doi:10.1016/j.talanta.2020.121638

A new highly enriched ²³³U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

Richard M. Essex, Ross W. Williams, Kayron T. Rogers, Cole R. Hexel, Tashi Parsons-Davis, Kerri C. Treinen

Chemical & Isotopic Mass Spectrometry

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

6 Scopus citations

Abstract

A highly-enriched ²³³U reference material (>0.99987 n(²³³U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity ²³³U to further reduce trace amounts of contaminant Pu in the material. The purified ²³³U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used ²³³U certified reference materials.

Original language	English
Article number	121638
Journal	Talanta
Volume	221
DOIs	https://doi.org/10.1016/j.talanta.2020.121638
State	Published - Jan 1 2021

Funding

Assistance from Joseph Giaquinto at ORNL and Paul Croatto at the United States Department of Energy was instrumental to the successful completion of this project. Funding for the characterization work at LLNL and ORNL and project coordination activities at NIST was provided by the United States Department of Homeland Security . The starting material for this project was made available through a project funded by the NNSA. To enhance measurement capabilities for sample-limited analyses of uranium, a collaborative project was initiated by the United States Department of Homeland Security (DHS) and the National Nuclear Security Administration (NNSA) to produce a very highly enriched 233U isotope dilution mass spectrometry reference material (henceforth referred to as the U-233 Spike). The starting material for the U-233 Spike, UTHX001-A, was provided from a stock of legacy 233U material preserved by NNSA [21] and stored at Oak Ridge National Laboratory (ORNL). DHS supported project coordination by staff at the National Institute of Standards and Technology (NIST) and preparation and characterization of the reference material at Lawrence Livermore National Laboratory (LLNL) and ORNL.Assistance from Joseph Giaquinto at ORNL and Paul Croatto at the United States Department of Energy was instrumental to the successful completion of this project. Funding for the characterization work at LLNL and ORNL and project coordination activities at NIST was provided by the United States Department of Homeland Security. The starting material for this project was made available through a project funded by the NNSA.

Funders	Funder number
Joseph Giaquinto
U.S. Department of Homeland Security
Department of Human Services
National Nuclear Security Administration
Lawrence Livermore National Laboratory
Oak Ridge National Laboratory

Keywords

Isotope amount ratio
Isotope dilution mass spectrometry
Modified Davies and Gray titration
Nuclear forensics
Nuclear safeguards
U
Uranium

Access to Document

10.1016/j.talanta.2020.121638

Cite this

@article{0cd5dec5521b4fbd96a9fc12294adc3d,

title = "A new highly enriched 233U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples",

abstract = "A highly-enriched 233U reference material (>0.99987 n(233U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233U to further reduce trace amounts of contaminant Pu in the material. The purified 233U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233U certified reference materials.",

keywords = "Isotope amount ratio, Isotope dilution mass spectrometry, Modified Davies and Gray titration, Nuclear forensics, Nuclear safeguards, U, Uranium",

author = "Essex, {Richard M.} and Williams, {Ross W.} and Rogers, {Kayron T.} and Hexel, {Cole R.} and Tashi Parsons-Davis and Treinen, {Kerri C.}",

note = "Publisher Copyright: {\textcopyright} 2020",

year = "2021",

month = jan,

day = "1",

doi = "10.1016/j.talanta.2020.121638",

language = "English",

volume = "221",

journal = "Talanta",

issn = "0039-9140",

publisher = "Elsevier",

}

TY - JOUR

T1 - A new highly enriched 233U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

AU - Essex, Richard M.

AU - Williams, Ross W.

AU - Rogers, Kayron T.

AU - Hexel, Cole R.

AU - Parsons-Davis, Tashi

AU - Treinen, Kerri C.

PY - 2021/1/1

Y1 - 2021/1/1

N2 - A highly-enriched 233U reference material (>0.99987 n(233U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233U to further reduce trace amounts of contaminant Pu in the material. The purified 233U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233U certified reference materials.

AB - A highly-enriched 233U reference material (>0.99987 n(233U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233U to further reduce trace amounts of contaminant Pu in the material. The purified 233U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233U certified reference materials.

KW - Isotope amount ratio

KW - Isotope dilution mass spectrometry

KW - Modified Davies and Gray titration

KW - Nuclear forensics

KW - Nuclear safeguards

KW - U

KW - Uranium

UR - http://www.scopus.com/inward/record.url?scp=85091218767&partnerID=8YFLogxK

U2 - 10.1016/j.talanta.2020.121638

DO - 10.1016/j.talanta.2020.121638

M3 - Article

C2 - 33076158

AN - SCOPUS:85091218767

SN - 0039-9140

VL - 221

JO - Talanta

JF - Talanta

M1 - 121638

ER -