In Situ Raman Spectroscopy of Uranyl Peroxide Nanoscale Cage Clusters Under Hydrothermal Conditions
Abstract
Aqueous solutions containing the nanoscale uranyl peroxide cage clusters U60, [(UO2)(O2)(OH)]6060-, and U60Ox30, [{(UO2)(O2)}60(C2O4)30]60-, were monitored by in situ Raman spectroscopy during stepwise heating to 180°C. In solutions with U60, clusters persist to 120°C, although conversion of U60 to U24, [(UO2)(O2)(OH)]2424-, occurs above 100°C. U60Ox30 persisted in solutions heated to 150°C, although partial conversion to smaller uranyl peroxide clusters species was observed beginning at 100°C. Upon breakdown of the uranyl peroxide cage clusters, uranium precipitated as a compreignacite-like phase, K2[(UO2)3O2(OH)3]2(H2O)7, and metaschoepite, [(UO2)8O2(OH)12](H2O)10. In this work, the role of the countercations, oxalate bridge, and solution pH are examined in order to better understand the mobility of these species at elevated temperatures.
- Authors:
-
- Univ. of Notre Dame, Notre Dame, IN (United States)
- McGill Univ., Montreal, QC (Canada)
- Salem State Univ., Salem, MA (United States)
- Publication Date:
- Research Org.:
- Univ. of Notre Dame, IN (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1510719
- Alternate Identifier(s):
- OSTI ID: 1511506
- Grant/Contract Number:
- NA0003763
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Dalton Transactions
- Additional Journal Information:
- Journal Volume: 48; Journal Issue: 22; Journal ID: ISSN 1477-9226
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Lobeck, Haylie, Traustason, Hrafn, Julien, Patrick, Fitzpatrick, John, Mana, Sara, Szymanowski, Jennifer, and Burns, Peter C. In Situ Raman Spectroscopy of Uranyl Peroxide Nanoscale Cage Clusters Under Hydrothermal Conditions. United States: N. p., 2019.
Web. doi:10.1039/C9DT01529A.
Lobeck, Haylie, Traustason, Hrafn, Julien, Patrick, Fitzpatrick, John, Mana, Sara, Szymanowski, Jennifer, & Burns, Peter C. In Situ Raman Spectroscopy of Uranyl Peroxide Nanoscale Cage Clusters Under Hydrothermal Conditions. United States. https://doi.org/10.1039/C9DT01529A
Lobeck, Haylie, Traustason, Hrafn, Julien, Patrick, Fitzpatrick, John, Mana, Sara, Szymanowski, Jennifer, and Burns, Peter C. Tue .
"In Situ Raman Spectroscopy of Uranyl Peroxide Nanoscale Cage Clusters Under Hydrothermal Conditions". United States. https://doi.org/10.1039/C9DT01529A. https://www.osti.gov/servlets/purl/1510719.
@article{osti_1510719,
title = {In Situ Raman Spectroscopy of Uranyl Peroxide Nanoscale Cage Clusters Under Hydrothermal Conditions},
author = {Lobeck, Haylie and Traustason, Hrafn and Julien, Patrick and Fitzpatrick, John and Mana, Sara and Szymanowski, Jennifer and Burns, Peter C.},
abstractNote = {Aqueous solutions containing the nanoscale uranyl peroxide cage clusters U60, [(UO2)(O2)(OH)]6060-, and U60Ox30, [{(UO2)(O2)}60(C2O4)30]60-, were monitored by in situ Raman spectroscopy during stepwise heating to 180°C. In solutions with U60, clusters persist to 120°C, although conversion of U60 to U24, [(UO2)(O2)(OH)]2424-, occurs above 100°C. U60Ox30 persisted in solutions heated to 150°C, although partial conversion to smaller uranyl peroxide clusters species was observed beginning at 100°C. Upon breakdown of the uranyl peroxide cage clusters, uranium precipitated as a compreignacite-like phase, K2[(UO2)3O2(OH)3]2(H2O)7, and metaschoepite, [(UO2)8O2(OH)12](H2O)10. In this work, the role of the countercations, oxalate bridge, and solution pH are examined in order to better understand the mobility of these species at elevated temperatures.},
doi = {10.1039/C9DT01529A},
journal = {Dalton Transactions},
number = 22,
volume = 48,
place = {United States},
year = {Tue Jan 01 00:00:00 EST 2019},
month = {Tue Jan 01 00:00:00 EST 2019}
}
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