Effects of H2O2 Concentration on Formation of Uranyl Peroxide Species Probed by Dissolution of Uranium Nitride and Uranium Dioxide

Hickam, Sarah; Breier, Jaclyn; Cripe, Yasmeen; Cole, Erica; Burns, Peter C.

doi:10.1021/acs.inorgchem.9b00231

Title: Effects of H₂O₂ Concentration on Formation of Uranyl Peroxide Species Probed by Dissolution of Uranium Nitride and Uranium Dioxide

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Abstract

Dissolution of uranium materials in alkaline aqueous conditions containing H₂O₂ results in uranyl peroxide species in solution, including anionic uranyl peroxide cage clusters. Uranyl peroxide cage clusters are generally highly soluble in water, where they persist as aqueous macroanions. Previous studies indicate that uranyl cluster speciation and dissolution of uranium materials is impacted by the concentration of alkali metal in solution, but in these studies, high concentrations of H₂O₂ were used. Herein, the role of hydrogen peroxide concentration is examined relative to the dissolution of powdered UN and UO₂. Lower initial H₂O₂ concentrations reduce dissolution of UO₂ and UN and tend to produce simple (small) uranyl peroxide species rather the highly soluble uranyl peroxide clusters. H₂O₂ availability will have implications for uranyl speciation and solubility where spent nuclear fuel is in contact with water and where alkaline peroxide conditions are used in dissolution of nuclear material.

Authors:

Hickam, Sarah ^[1]; Breier, Jaclyn ^[1]; Cripe, Yasmeen ^[1]; Cole, Erica ^[1];

^[2]

Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences
Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences, and Dept. of Chemistry and Biochemistry

Publication Date:: Tue Apr 09 00:00:00 EDT 2019

Research Org.:: Univ. of Notre Dame, IN (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1506972

Grant/Contract Number:: NA0003763

Resource Type:: Accepted Manuscript

Journal Name:: Inorganic Chemistry

Additional Journal Information:: Journal Volume: 58; Journal Issue: 9; Journal ID: ISSN 0020-1669

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Hickam, Sarah, Breier, Jaclyn, Cripe, Yasmeen, Cole, Erica, and Burns, Peter C. Effects of H2O2 Concentration on Formation of Uranyl Peroxide Species Probed by Dissolution of Uranium Nitride and Uranium Dioxide.  United States: N. p., 2019. 
Web.  doi:10.1021/acs.inorgchem.9b00231.

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                    Hickam, Sarah, Breier, Jaclyn, Cripe, Yasmeen, Cole, Erica, & Burns, Peter C. Effects of H2O2 Concentration on Formation of Uranyl Peroxide Species Probed by Dissolution of Uranium Nitride and Uranium Dioxide.  United States.  https://doi.org/10.1021/acs.inorgchem.9b00231

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                    Hickam, Sarah, Breier, Jaclyn, Cripe, Yasmeen, Cole, Erica, and Burns, Peter C. Tue .  
"Effects of H2O2 Concentration on Formation of Uranyl Peroxide Species Probed by Dissolution of Uranium Nitride and Uranium Dioxide".  United States.  https://doi.org/10.1021/acs.inorgchem.9b00231.  https://www.osti.gov/servlets/purl/1506972.

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@article{osti_1506972,

  title        = {Effects of H2O2 Concentration on Formation of Uranyl Peroxide Species Probed by Dissolution of Uranium Nitride and Uranium Dioxide},

  author       = {Hickam, Sarah and Breier, Jaclyn and Cripe, Yasmeen and Cole, Erica and Burns, Peter C.},

  abstractNote = {Dissolution of uranium materials in alkaline aqueous conditions containing H2O2 results in uranyl peroxide species in solution, including anionic uranyl peroxide cage clusters. Uranyl peroxide cage clusters are generally highly soluble in water, where they persist as aqueous macroanions. Previous studies indicate that uranyl cluster speciation and dissolution of uranium materials is impacted by the concentration of alkali metal in solution, but in these studies, high concentrations of H2O2 were used. Herein, the role of hydrogen peroxide concentration is examined relative to the dissolution of powdered UN and UO2. Lower initial H2O2 concentrations reduce dissolution of UO2 and UN and tend to produce simple (small) uranyl peroxide species rather the highly soluble uranyl peroxide clusters. H2O2 availability will have implications for uranyl speciation and solubility where spent nuclear fuel is in contact with water and where alkaline peroxide conditions are used in dissolution of nuclear material.},

  doi          = {10.1021/acs.inorgchem.9b00231},

  journal      = {Inorganic Chemistry},

  number       = 9,

  volume       = 58,

  place        = {United States},

  year         = {Tue Apr 09 00:00:00 EDT 2019},

  month        = {Tue Apr 09 00:00:00 EDT 2019}

}

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Title: Effects of H2O2 Concentration on Formation of Uranyl Peroxide Species Probed by Dissolution of Uranium Nitride and Uranium Dioxide

Abstract

Citation Formats

Title: Effects of H₂O₂ Concentration on Formation of Uranyl Peroxide Species Probed by Dissolution of Uranium Nitride and Uranium Dioxide