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Issue 22, 2019
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In situ Raman spectroscopy of uranyl peroxide nanoscale cage clusters under hydrothermal conditions

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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 containing 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. 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.

Graphical abstract: In situ Raman spectroscopy of uranyl peroxide nanoscale cage clusters under hydrothermal conditions

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Supplementary files

Article information


Submitted
10 Apr 2019
Accepted
30 Apr 2019
First published
30 Apr 2019

Dalton Trans., 2019,48, 7755-7765
Article type
Paper
Author version available

In situ Raman spectroscopy of uranyl peroxide nanoscale cage clusters under hydrothermal conditions

H. L. Lobeck, H. Traustason, P. A. Julien, J. R. FitzPatrick, S. Mana, J. E. S. Szymanowski and P. C. Burns, Dalton Trans., 2019, 48, 7755
DOI: 10.1039/C9DT01529A

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