An approach to separating Pu, U, and Ti from high-purity graphite for isotopic analysis by MC-ICP-MS

Metzger, Shalina; Manard, Benjamin; Bostick, Debra; Ticknor, Brian; Rogers, Kayron; Mcbay, Eddie; Glasgow, David; Zirakparvar, N; Hexel, Cole

doi:10.1039/D1JA00079A

An approach to separating Pu, U, and Ti from high-purity graphite for isotopic analysis by MC-ICP-MS

Journal Article · Mon Apr 19 00:00:00 EDT 2021 · Journal of Analytical Atomic Spectrometry

DOI:https://doi.org/10.1039/D1JA00079A· OSTI ID:1785216

^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Div.

Information about elemental and isotopic systematics of ultra-trace level actinides (e.g. U and Pu) and main group elements (e.g. Ti) present within nuclear grade graphite is vital to the nuclear community for improved reactor operation and security. In support of this, extensive effort has been placed on improving analysis methods (i.e., inductively coupled plasma-mass spectrometry). However, significantly less effort has been devoted to the optimization of chemical separation methods. Within the separation community, commercially available Eichrom™ resins are often employed, as their elution characteristics for various elements have been well studied, but the direct optimization of actinides and trace metal separations from a single sample have not been widely investigated. Here, methods using various Eichrom pre-packed cartridges were explored to achieve separation of ultra-trace levels of U, Pu, and Ti from a variety of graphite samples. Once the validity of the combined separation scheme was established using certified reference materials, the method was applied to historic, unirradiated and irradiated, graphite samples. For all samples investigated, precise isotope ratio measurements for the titanium isotope systems were made.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1785216

Alternate ID(s):: OSTI ID: 1779990

Journal Information:: Journal of Analytical Atomic Spectrometry, Journal Name: Journal of Analytical Atomic Spectrometry Vol. 36; ISSN 0267-9477

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (39)

Accurate and precise determination of isotopic ratios by MC-ICP-MS: A review Yang, Lu Mass Spectrometry Reviews, Vol. 28, Issue 6 https://doi.org/10.1002/mas.20251	journal	November 2009
Pure graphite as a reference material for the determination of trace elements — an interlaboratory collaborative study Bögershausen, W.; Cicciarelli, R.; Gercken, B. Fresenius Journal of Analytical Chemistry, Vol. 357, Issue 3 https://doi.org/10.1007/s002160050151	journal	February 1997
Trace analysis of high-purity graphite by LA-ICP-MS Pickhardt, Carola; Becker, Johanna Sabine Fresenius' Journal of Analytical Chemistry, Vol. 370, Issue 5 https://doi.org/10.1007/s002160100873	journal	July 2001
Chemical characterization of graphite by instrumental neutron activation analysis Shinde, Amol D.; Acharya, R.; Verma, R. Journal of Radioanalytical and Nuclear Chemistry, Vol. 294, Issue 3 https://doi.org/10.1007/s10967-011-1467-2	journal	October 2011
Determination of concentrations of trace elements in nuclear grade graphite by charged particle activation analysis Datta, J.; Chowdhury, D. P.; Verma, R. Journal of Radioanalytical and Nuclear Chemistry, Vol. 300, Issue 1 https://doi.org/10.1007/s10967-014-2977-5	journal	February 2014
Separation and preconcentration of uranium from acidic media by extraction chromatography Horwitz, E. Philip; Dietz, Mark L.; Chiarizia, Renato Analytica Chimica Acta, Vol. 266, Issue 1 https://doi.org/10.1016/0003-2670(92)85276-C	journal	August 1992
Separation and preconcentration of actinides by extraction chromatography using a supported liquid anion exchanger: application to the characterization of high-level nuclear waste solutions Horwitz, E. Philip; Dietz, Mark L.; Chiarizia, Renato Analytica Chimica Acta, Vol. 310, Issue 1 https://doi.org/10.1016/0003-2670(95)00144-O	journal	June 1995
Graphite as a neutron moderator and reflector material Baker, D. E. Nuclear Engineering and Design, Vol. 14, Issue 3 https://doi.org/10.1016/0029-5493(70)90160-3	journal	February 1971
Laser ablation inductively coupled plasma mass spectrometry for the trace, ultratrace and isotope analysis of long-lived radionuclides in solid samples Becker, Johanna Sabine; Pickhardt, Carola; Dietze, Hans-Joachim International Journal of Mass Spectrometry, Vol. 202, Issue 1-3 https://doi.org/10.1016/S1387-3806(00)00251-7	journal	October 2000
High precision measurement of titanium isotope ratios by plasma source mass spectrometry Zhu, X. K.; Makishima, A.; Guo, Y. International Journal of Mass Spectrometry, Vol. 220, Issue 1 https://doi.org/10.1016/S1387-3806(02)00767-4	journal	September 2002
Determination of impurities in graphite using synchrotron radiation based X-ray fluorescence spectrometry Ghosh, M.; Swain, K. K.; Remya Devi, P. S. Applied Radiation and Isotopes, Vol. 128 https://doi.org/10.1016/j.apradiso.2017.07.025	journal	October 2017
A review on solid phase extraction of actinides and lanthanides with amide based extractants Ansari, Seraj A.; Mohapatra, Prasanta K. Journal of Chromatography A, Vol. 1499 https://doi.org/10.1016/j.chroma.2017.03.035	journal	May 2017
Titanium isotopes and rare earth patterns in CAIs: Evidence for thermal processing and gas-dust decoupling in the protoplanetary disk Davis, Andrew M.; Zhang, Junjun; Greber, Nicolas D. Geochimica et Cosmochimica Acta, Vol. 221 https://doi.org/10.1016/j.gca.2017.07.032	journal	January 2018
High precision titanium isotope measurements on geological samples by high resolution MC-ICPMS Leya, Ingo; Schönbächler, Maria; Wiechert, Uwe International Journal of Mass Spectrometry, Vol. 262, Issue 3 https://doi.org/10.1016/j.ijms.2006.12.001	journal	May 2007
Exploration of ICP platforms for measuring elemental impurities in uranium ore concentrates Manard, Benjamin T.; Metzger, Shalina C.; Rogers, Kayron T. International Journal of Mass Spectrometry, Vol. 455 https://doi.org/10.1016/j.ijms.2020.116378	journal	September 2020
Separation of actinides from spent nuclear fuel: A review Veliscek-Carolan, Jessica Journal of Hazardous Materials, Vol. 318 https://doi.org/10.1016/j.jhazmat.2016.07.027	journal	November 2016
Microwave-induced combustion method for the determination of trace and ultratrace element impurities in graphite samples by ICP-OES and ICP-MS Cruz, Sandra M.; Schmidt, Lucas; Dalla Nora, Flavia M. Microchemical Journal, Vol. 123 https://doi.org/10.1016/j.microc.2015.05.008	journal	November 2015
Direct atomic absorption spectrometry determination of tin, lead, cadmium and zinc in high-purity graphite with flame furnace atomizer☆ Zacharia, A.; Gucer, S.; Izgi, B. Talanta, Vol. 72, Issue 2 https://doi.org/10.1016/j.talanta.2006.10.040	journal	April 2007
Optimization of uranium and plutonium separations using TEVA and UTEVA cartridges for MC-ICP-MS analysis of environmental swipe samples Metzger, Shalina C.; Rogers, Kayron T.; Bostick, Debra A. Talanta, Vol. 198 https://doi.org/10.1016/j.talanta.2019.02.034	journal	June 2019
Investigation of Impurities of RBMK Graphite by Different Methods Plukienė, Rita; Lagzdina, Elena; Juodis, Laurynas Radiocarbon, Vol. 60, Issue 6 https://doi.org/10.1017/RDC.2018.93	journal	November 2018
Analysis of high-purity graphite for trace elements by inductively coupled plasma atomic emission spectrometry after chelating resin preconcentration Mahanti, Himansu S.; Barnes, Ramon M. Analytical Chemistry, Vol. 55, Issue 2 https://doi.org/10.1021/ac00253a059	journal	February 1983
Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry Metzger, Shalina C.; Ticknor, Brian W.; Rogers, Kayron T. Analytical Chemistry, Vol. 90, Issue 15 https://doi.org/10.1021/acs.analchem.8b02095	journal	June 2018
Isobaric Spike Method for Absolute Isotopic Ratio Determination by MC-ICP-MS Shuai, Kang; Li, Weiqiang; Hui, Hejiu Analytical Chemistry, Vol. 92, Issue 7 https://doi.org/10.1021/acs.analchem.9b04160	journal	February 2020
Determination of impurity elements in graphite by acid decomposition–inductively coupled plasma atomic emission spectrometry Watanabe, Kazuo; Inagawa, Jun The Analyst, Vol. 121, Issue 5 https://doi.org/10.1039/AN9962100623	journal	January 1996
Ultra-precise titanium stable isotope measurements by double-spike high resolution MC-ICP-MS Millet, Marc-Alban; Dauphas, Nicolas Journal of Analytical Atomic Spectrometry, Vol. 29, Issue 8 https://doi.org/10.1039/C4JA00096J	journal	January 2014
Mass spectrometric analysis for nuclear safeguards Boulyga, Sergei; Konegger-Kappel, Stefanie; Richter, Stephan Journal of Analytical Atomic Spectrometry, Vol. 30, Issue 7 https://doi.org/10.1039/C4JA00491D	journal	January 2015
Thermal ionisation mass spectrometry (TIMS) in nuclear science and technology – a review Aggarwal, Suresh K. Analytical Methods, Vol. 8, Issue 5 https://doi.org/10.1039/C5AY02816G	journal	January 2016
Critical need for plutonium and uranium isotopic standards with lower uncertainties Mathew, Kattathu J.; Stanley, Floyd E.; Thomas, Mariam R. Analytical Methods, Vol. 8, Issue 40 https://doi.org/10.1039/C6AY02267G	journal	January 2016
Uranium isotope analysis by MC-ICP-MS in sub-ng sized samples Boulyga, Sergei F.; Koepf, Andreas; Konegger-Kappel, Stefanie Journal of Analytical Atomic Spectrometry, Vol. 31, Issue 11 https://doi.org/10.1039/C6JA00238B	journal	January 2016
Multi-element ion-exchange chromatography and high-precision MC-ICP-MS isotope analysis of Mg and Ti from sub-mm-sized meteorite inclusions Larsen, K. K.; Wielandt, D.; Bizzarro, M. Journal of Analytical Atomic Spectrometry, Vol. 33, Issue 4 https://doi.org/10.1039/C7JA00392G	journal	January 2018
Combination of ⁴⁷ Ti and ⁴⁸ Ti for the determination of highly polydisperse TiO ₂ particle size distributions by spICP-MS Bucher, Guillaume; Auger, François Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 7 https://doi.org/10.1039/C9JA00101H	journal	January 2019
Determination of impurity elements in high purity graphite by inductively coupled plasma atomic emission spectrometry after microwave decomposition Watanabe, Mitsuyoshi; Narukawa, Akira The Analyst, Vol. 125, Issue 6 https://doi.org/10.1039/b001608j	journal	January 2000
Optimisation and application of ICP-MS and alpha-spectrometry for determination of isotopic ratios of depleted uranium and plutonium in samples collected in Kosovo Boulyga, Sergei F.; Testa, Corrado; Desideri, Donatella Journal of Analytical Atomic Spectrometry, Vol. 16, Issue 11, p. 1283-1289 https://doi.org/10.1039/b103178n	journal	October 2001
Separation of titanium from silicates for isotopic ratio determination using multiple collector ICP-MS Makishima, Akio; Zhu, Xiang-Kun; Belshaw, Nick S. Journal of Analytical Atomic Spectrometry, Vol. 17, Issue 10 https://doi.org/10.1039/b204349a	journal	July 2002
A new method for MC-ICPMS measurement of titanium isotopic composition: Identification of correlated isotope anomalies in meteorites Zhang, Junjun; Dauphas, Nicolas; Davis, Andrew M. Journal of Analytical Atomic Spectrometry, Vol. 26, Issue 11 https://doi.org/10.1039/c1ja10181a	journal	January 2011
Isotopic Depletion and Decay Methods and Analysis Capabilities in SCALE Gauld, Ian C.; Radulescu, Georgeta; Ilas, Germina Nuclear Technology, Vol. 174, Issue 2 https://doi.org/10.13182/NT11-3	journal	May 2011
Direct Determination of Trace Elements in Graphite Matrices Using Modulated Glow Discharge Atomic Absorption Spectrometry Pan, Changkang; King, Fred L. Applied Spectroscopy, Vol. 47, Issue 3 https://doi.org/10.1366/0003702934066730	journal	March 1993
Isotopic compositions of the elements 2013 (IUPAC Technical Report) Meija, Juris; Coplen, Tyler B.; Berglund, Michael Pure and Applied Chemistry, Vol. 88, Issue 3 https://doi.org/10.1515/pac-2015-0503	journal	March 2016
Mass spectrometric determination of impurities in reactor core graphite for radioactive waste composition modelling Puzas, A.; Remeikis, V.; Ežerinskis, Ž. Lithuanian Journal of Physics, Vol. 50, Issue 4 https://doi.org/10.3952/lithjphys.50412	journal	January 2010

Similar Records

Optimization of uranium and plutonium separations using TEVA and UTEVA cartridges for MC-ICP-MS analysis of environmental swipe samples

Journal Article · Tue Feb 05 19:00:00 EST 2019 · Talanta · OSTI ID:1494892

NEW METHOD FOR DETERMINATION OF ACTINIDES AND STRONTIUM IN ANIMAL TISSUE

Journal Article · Mon May 07 00:00:00 EDT 2007 · Journal of Radioanlytical and Nuclear Chemistry · OSTI ID:903100

Rapid Column Extraction Method for Actinides and Sr-89/90 in Water Samples

Journal Article · Wed Jun 15 00:00:00 EDT 2005 · OSTI ID:881365

Related Subjects

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
Graphite
MC-ICP-MS
Plutonium
Separations
Titanium
Uranium

An approach to separating Pu, U, and Ti from high-purity graphite for isotopic analysis by MC-ICP-MS

Citation Formats

References (39)

Similar Records

Related Subjects