skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: In Situ Raman Spectroscopy of Uranyl Peroxide Nanoscale Cage Clusters Under Hydrothermal Conditions

Abstract

Aqueous solutions containing the nanoscale uranyl peroxide cage clusters U 60, [(UO 2)(O 2)(OH)] 60 60-, and U 60Ox 30, [{(UO 2)(O 2)} 60(C 2O 4) 30] 60-, were monitored by in situ Raman spectroscopy during stepwise heating to 180°C. In solutions with U 60, clusters persist to 120°C, although conversion of U 60 to U 24, [(UO 2)(O 2)(OH)] 24 24-, occurs above 100°C. U 60Ox 30 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, K 2[(UO 2) 3O 2(OH) 3] 2(H 2O) 7, and metaschoepite, [(UO 2) 8O 2(OH) 12](H 2O) 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:
 [1];  [1];  [2];  [1];  [3];  [1];  [1]
  1. Univ. of Notre Dame, Notre Dame, IN (United States)
  2. McGill Univ., Montreal, QC (Canada)
  3. Salem State Univ., Salem, MA (United States)
Publication Date:
Research Org.:
Univ. of Notre Dame, 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:
Journal Article: Accepted Manuscript
Journal Name:
Dalton Transactions
Additional Journal Information:
Journal Name: Dalton Transactions; 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. doi: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. doi:10.1039/C9DT01529A.
@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},
issn = {1477-9226},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on January 1, 2020
Publisher's Version of Record

Save / Share: