Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins

Mastren, Tara; Stein, Benjamin W.; Parker, T. Gannon; Radchenko, Valery; Copping, Roy; Owens, Allison; Wyant, Lance E.; Brugh, Mark; Kozimor, Stosh A.; Nortier, F. Meiring; Birnbaum, Eva R.; John, Kevin D.; Fassbender, Michael E.

doi:10.1021/acs.analchem.8b01380

Title: Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins

Abstract

Protactinium-230 (t_1/2 = 17.4 d) is the parent isotope of ²³⁰U (t_1/2 = 20.8 d), a radionuclide of interest for targeted alpha therapy (TAT). Column chromatographic methods have been developed to separate no-carrier-added ²³⁰Pa from proton irradiated thorium targets and accompanying fission products. Results reported within this paper demonstrate the use of novel sulfur bearing chromatographic extraction resins for the selective separation of protactinium. The recovery yield of ²³⁰Pa was 93 ± 4% employing a R₃P=S type commercially available resin and 88 ± 4% employing a DGTA (diglycothioamide) containing custom synthesized extraction chromatographic resin. The radiochemical purity of the recovered ²³⁰Pa was measured via high purity germanium γ-ray spectroscopy to be >99.5% with the remaining radioactive contaminant being ⁹⁵Nb due to its similar chemistry to protactinium. Finally, measured equilibrium distribution coefficients for protactinium, thorium, uranium, niobium, radium, and actinium on both the R₃P=S type and the DGTA resin in hydrochloric acid media are reported, to the best of our knowledge, for the first time.

Authors:

Mastren, Tara ^[1]; Stein, Benjamin W. ^[1]; Parker, T. Gannon ^[1]; Radchenko, Valery ^[1]; Copping, Roy ^[2]; Owens, Allison ^[2]; Wyant, Lance E. ^[2]; Brugh, Mark ^[1]; Kozimor, Stosh A. ^[1]; Nortier, F. Meiring ^[1]; Birnbaum, Eva R. ^[1]; John, Kevin D. ^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Nuclear Security and Isotope Technology Division

Publication Date:: 2018-05-14

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Nuclear Physics (NP)

OSTI Identifier:: 1440455

Alternate Identifier(s):: OSTI ID: 1842640

Report Number(s):: LA-UR-18-22616
Journal ID: ISSN 0003-2700; TRN: US1900741

Grant/Contract Number:: AC52-06NA25396; AC05-00OR22725

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Analytical Chemistry

Additional Journal Information:: Journal Volume: 90; Journal Issue: 11; Journal ID: ISSN 0003-2700

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Uranium; Organic polymers; Chromatography; Thorium; Extraction

Citation Formats


                    Mastren, Tara, Stein, Benjamin W., Parker, T. Gannon, Radchenko, Valery, Copping, Roy, Owens, Allison, Wyant, Lance E., Brugh, Mark, Kozimor, Stosh A., Nortier, F. Meiring, Birnbaum, Eva R., John, Kevin D., and Fassbender, Michael E.. Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins.  United States: N. p., 2018. 
        Web.  doi:10.1021/acs.analchem.8b01380.

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                    Mastren, Tara, Stein, Benjamin W., Parker, T. Gannon, Radchenko, Valery, Copping, Roy, Owens, Allison, Wyant, Lance E., Brugh, Mark, Kozimor, Stosh A., Nortier, F. Meiring, Birnbaum, Eva R., John, Kevin D., & Fassbender, Michael E.. Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins.  United States.  https://doi.org/10.1021/acs.analchem.8b01380

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                    Mastren, Tara, Stein, Benjamin W., Parker, T. Gannon, Radchenko, Valery, Copping, Roy, Owens, Allison, Wyant, Lance E., Brugh, Mark, Kozimor, Stosh A., Nortier, F. Meiring, Birnbaum, Eva R., John, Kevin D., and Fassbender, Michael E.. 2018.  
        "Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins".  United States.  https://doi.org/10.1021/acs.analchem.8b01380.  https://www.osti.gov/servlets/purl/1440455.

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@article{osti_1440455,

  title        = {Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins},

  author       = {Mastren, Tara and Stein, Benjamin W. and Parker, T. Gannon and Radchenko, Valery and Copping, Roy and Owens, Allison and Wyant, Lance E. and Brugh, Mark and Kozimor, Stosh A. and Nortier, F. Meiring and Birnbaum, Eva R. and John, Kevin D. and Fassbender, Michael E.},

  abstractNote = {Protactinium-230 (t1/2 = 17.4 d) is the parent isotope of 230U (t1/2 = 20.8 d), a radionuclide of interest for targeted alpha therapy (TAT). Column chromatographic methods have been developed to separate no-carrier-added 230Pa from proton irradiated thorium targets and accompanying fission products. Results reported within this paper demonstrate the use of novel sulfur bearing chromatographic extraction resins for the selective separation of protactinium. The recovery yield of 230Pa was 93 ± 4% employing a R3P=S type commercially available resin and 88 ± 4% employing a DGTA (diglycothioamide) containing custom synthesized extraction chromatographic resin. The radiochemical purity of the recovered 230Pa was measured via high purity germanium γ-ray spectroscopy to be >99.5% with the remaining radioactive contaminant being 95Nb due to its similar chemistry to protactinium. Finally, measured equilibrium distribution coefficients for protactinium, thorium, uranium, niobium, radium, and actinium on both the R3P=S type and the DGTA resin in hydrochloric acid media are reported, to the best of our knowledge, for the first time.},

  doi          = {10.1021/acs.analchem.8b01380},

  url          = {https://www.osti.gov/biblio/1440455},
  journal      = {Analytical Chemistry},

  issn         = {0003-2700},

  number       = 11,

  volume       = 90,

  place        = {United States},

  year         = {2018},

  month        = {5}

}

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https://doi.org/10.1021/acs.analchem.8b01380

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Cited by: 15 works

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Figure 1: Decay scheme of ²³⁰Pa.

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Similar Records

Title: Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins

Abstract

Citation Formats

Figures / Tables:

and contamination at zero age: a possible limitation on U/Th series dating of speleothem material journal, April 1999

Elucidating Protactinium Hydrolysis: The Relative Stabilities of PaO 2 (H 2 O) + and PaO(OH) 2 + journal, July 2015

Extraction and separation of thorium(IV) and protactinium(V) by 2-carbethoxy-5-hydroxy-1-(4-tolyl)-4-pyridone journal, August 1972

Actinide Partitioning—A Review journal, May 2001

Formation cross-sections and chromatographic separation of protactinium isotopes formed in proton-irradiated thorium metal journal, January 2016

Mechanism of Trivalent Actinide/Lanthanide Separation Using Bis(2,4,4-Trimethylpentyl) Dithiophosphinic acid (Cyanex 301) and Neutral O-Bearing Co-Extractant Synergistic Mixtures journal, May 2001

Spectroscopic and computational investigation of actinium coordination chemistry journal, August 2016

Age Determination of Highly Enriched Uranium: Separation and Analysis of 231 Pa journal, November 2002

A simple-rapid method to separate uranium, thorium, and protactinium for U-series age-dating of materials journal, August 2014

Equilibrium core design methods for molten salt breeder reactor based on two-cell model journal, July 2015

Cross-sections of the reaction 232Th(p,3n)230Pa for production of 230U for targeted alpha therapy journal, October 2008

Organic carbon decomposition rates in sediments of the pacific manganese nodule belt dated by 230Th and 231Pa journal, November 1980

Sorption of Trace Heavy Metals by Thiol Containing Chelating Resins journal, January 2000

Covalency in f-element complexes journal, January 2013

Metal ion extraction with a thiol hydrophilic resin journal, October 1981

The Solvent Extraction of Protactinium journal, March 1956

Separation of Uranium and Protactinium from Thorium by Amine Extraction journal, May 1960

Protactinium—I analytical separations journal, January 1956

Novel Extraction of Chromatographic Resins Based on Tetraalkyldiglycolamides: Characterization and Potential Applications journal, May 2005

Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes journal, February 2015

Quantitative Radiochemical Analysis by Ion Exchange. Anion Exchange Behavior of Several Metal Ions in Hydrochloric, Nitric, and Sulfuric Acid Solutions journal, March 1959

Association constants of anionic-protactinium (V) complexes journal, March 1967

Separation of Thorium, Protactinium and Uranium by Ion Exchange and Extraction journal, August 1980

Production of 230 U/ 226 Th for Targeted Alpha Therapy via Proton Irradiation of 231 Pa journal, November 2008

Molten-Salt Reactor Chemistry journal, February 1970

Sorption of protactinium(V) on extraction chromatographic resins from nitric and hydrochloric solutions journal, September 2016

Antimicrobial activity of metals: mechanisms, molecular targets and applications journal, May 2013

EXTRACTION AND COEXTRACTION OF Tc(VII), Zr(IV), Np(IV.VI), Pa(V) AND Nb(V) WITH TRIBUTYL PHOSPHATE FROM NITRIC ACID SOLUTIONS journal, January 1989

Characterization of an extraction chromatographic resin for the separation and determination of 36Cl and 129I journal, August 2010

Possible Configurations for the Thorium Molten Salt Reactor and Advantages of the Fast Nonmoderated Version journal, January 2009

Extraction of Actinides(Iii), (Iv), (v), (Vi), and Lanthanides(Iii) by Structurally Tailored Diamides journal, February 2002

Comparative Studies on the Extraction of Protactinium Using Different Kinds of Organic Extractants journal, February 2009

Mercury(II) Adsorption from Wastewaters Using a Thiol Functional Adsorbent journal, April 2003

232Th(d,4n)230Pa cross-section measurements at ARRONAX facility for the production of 230U journal, May 2014

Extraction of palladium(II) from nitric acid solutions with diglycolthioamide journal, July 2015

Chromatographic separation of the theranostic radionuclide 111Ag from a proton irradiated thorium matrix journal, January 2018

Isolation and purification of protactinium-231 journal, April 2018

235U–231Pa age dating of uranium materials for nuclear forensic investigations journal, January 2013

Distribution coefficients of 60 elements on TODGA resin: Application to Ca, Lu, Hf, U and Th isotope geochemistry journal, May 2010

Extraction of protactinium from mineral acid-alcohol media journal, July 1968

Cross sections of the reaction Pa 231 ( d , 3 n ) U 230 for the production of U 230 / Th 226 for targeted α therapy journal, November 2009

Large scale accelerator production of 225Ac: Effective cross sections for 78–192 MeV protons incident on 232Th targets journal, December 2016

Determination of weight distribution ratios of Pa(V) and Np(V) with some extraction chromatography resins and the AG1-X8 resin journal, May 2013

Measurement of Attogram Quantities of 231 Pa in Dissolved and Particulate Fractions of Seawater by Isotope Dilution Thermal Ionization Mass Spectroscopy journal, March 2003

Trivalent minor actinides/lanthanides separation, using organophosphinic acids journal, June 1998

Liquid Fuel Molten Salt Reactors for Thorium Utilization journal, May 2016

231Pa dating of deep-sea cores via 227Th counting journal, December 1977

Observations of231Pa/235U disequilibrium in volcanic rocks journal, April 1997

Anion-exchange Studies. XXI. Th(IV) and U(IV) in Hydrochloric Acid. Separation of Thorium, Protactinium and Uranium 1,2 journal, June 1956

Investigation of para-sulfonatocalix[n]arenes [n = 6, 8] as potential chelates for 230 U journal, January 2010

Synthesis of symmetric dithiophosphinic acids for “minor actinide” extraction journal, June 2008

Microfluidics-based separation of actinium-225 from radium-225 for medical applications journal, May 2019

and contamination at zero age: a possible limitation on U/Th series dating of speleothem material
journal, April 1999

Elucidating Protactinium Hydrolysis: The Relative Stabilities of PaO ₂ (H ₂ O) ⁺ and PaO(OH) ₂ ⁺
journal, July 2015

Extraction and separation of thorium(IV) and protactinium(V) by 2-carbethoxy-5-hydroxy-1-(4-tolyl)-4-pyridone
journal, August 1972

Actinide Partitioning—A Review
journal, May 2001

Formation cross-sections and chromatographic separation of protactinium isotopes formed in proton-irradiated thorium metal
journal, January 2016

Mechanism of Trivalent Actinide/Lanthanide Separation Using Bis(2,4,4-Trimethylpentyl) Dithiophosphinic acid (Cyanex 301) and Neutral O-Bearing Co-Extractant Synergistic Mixtures
journal, May 2001

Spectroscopic and computational investigation of actinium coordination chemistry
journal, August 2016

Age Determination of Highly Enriched Uranium: Separation and Analysis of ²³¹ Pa
journal, November 2002

A simple-rapid method to separate uranium, thorium, and protactinium for U-series age-dating of materials
journal, August 2014

Equilibrium core design methods for molten salt breeder reactor based on two-cell model
journal, July 2015

Cross-sections of the reaction 232Th(p,3n)230Pa for production of 230U for targeted alpha therapy
journal, October 2008

Organic carbon decomposition rates in sediments of the pacific manganese nodule belt dated by 230Th and 231Pa
journal, November 1980

Sorption of Trace Heavy Metals by Thiol Containing Chelating Resins
journal, January 2000

Covalency in f-element complexes
journal, January 2013

Metal ion extraction with a thiol hydrophilic resin
journal, October 1981

The Solvent Extraction of Protactinium
journal, March 1956

Separation of Uranium and Protactinium from Thorium by Amine Extraction
journal, May 1960

Protactinium—I analytical separations
journal, January 1956

Novel Extraction of Chromatographic Resins Based on Tetraalkyldiglycolamides: Characterization and Potential Applications
journal, May 2005

Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes
journal, February 2015

Quantitative Radiochemical Analysis by Ion Exchange. Anion Exchange Behavior of Several Metal Ions in Hydrochloric, Nitric, and Sulfuric Acid Solutions
journal, March 1959

Association constants of anionic-protactinium (V) complexes
journal, March 1967

Separation of Thorium, Protactinium and Uranium by Ion Exchange and Extraction
journal, August 1980

Production of ²³⁰ U/ ²²⁶ Th for Targeted Alpha Therapy via Proton Irradiation of ²³¹ Pa
journal, November 2008

Molten-Salt Reactor Chemistry
journal, February 1970

Sorption of protactinium(V) on extraction chromatographic resins from nitric and hydrochloric solutions
journal, September 2016

Antimicrobial activity of metals: mechanisms, molecular targets and applications
journal, May 2013

EXTRACTION AND COEXTRACTION OF Tc(VII), Zr(IV), Np(IV.VI), Pa(V) AND Nb(V) WITH TRIBUTYL PHOSPHATE FROM NITRIC ACID SOLUTIONS
journal, January 1989

Characterization of an extraction chromatographic resin for the separation and determination of 36Cl and 129I
journal, August 2010

Possible Configurations for the Thorium Molten Salt Reactor and Advantages of the Fast Nonmoderated Version
journal, January 2009

Extraction of Actinides(Iii), (Iv), (v), (Vi), and Lanthanides(Iii) by Structurally Tailored Diamides
journal, February 2002

Comparative Studies on the Extraction of Protactinium Using Different Kinds of Organic Extractants
journal, February 2009

Mercury(II) Adsorption from Wastewaters Using a Thiol Functional Adsorbent
journal, April 2003

232Th(d,4n)230Pa cross-section measurements at ARRONAX facility for the production of 230U
journal, May 2014

Extraction of palladium(II) from nitric acid solutions with diglycolthioamide
journal, July 2015

Chromatographic separation of the theranostic radionuclide 111Ag from a proton irradiated thorium matrix
journal, January 2018

Isolation and purification of protactinium-231
journal, April 2018

235U–231Pa age dating of uranium materials for nuclear forensic investigations
journal, January 2013

Distribution coefficients of 60 elements on TODGA resin: Application to Ca, Lu, Hf, U and Th isotope geochemistry
journal, May 2010

Extraction of protactinium from mineral acid-alcohol media
journal, July 1968

Cross sections of the reaction ${}^{231}{Pa} (d, 3 n) {}^{230}U$ for the production of ${}^{230}U / {}^{226}{Th}$ for targeted $α$ therapy
journal, November 2009

Large scale accelerator production of 225Ac: Effective cross sections for 78–192 MeV protons incident on 232Th targets
journal, December 2016

Determination of weight distribution ratios of Pa(V) and Np(V) with some extraction chromatography resins and the AG1-X8 resin
journal, May 2013

Measurement of Attogram Quantities of ²³¹ Pa in Dissolved and Particulate Fractions of Seawater by Isotope Dilution Thermal Ionization Mass Spectroscopy
journal, March 2003

Trivalent minor actinides/lanthanides separation, using organophosphinic acids
journal, June 1998

Liquid Fuel Molten Salt Reactors for Thorium Utilization
journal, May 2016

231Pa dating of deep-sea cores via 227Th counting
journal, December 1977

Observations of231Pa/235U disequilibrium in volcanic rocks
journal, April 1997

Anion-exchange Studies. XXI. Th(IV) and U(IV) in Hydrochloric Acid. Separation of Thorium, Protactinium and Uranium ^1,2
journal, June 1956

Investigation of para-sulfonatocalix[n]arenes [n = 6, 8] as potential chelates for ²³⁰ U
journal, January 2010

Synthesis of symmetric dithiophosphinic acids for “minor actinide” extraction
journal, June 2008

Microfluidics-based separation of actinium-225 from radium-225 for medical applications
journal, May 2019