In situ Raman spectroscopy of uranyl peroxide nanoscale cage clusters under hydrothermal conditions
Autor: | Hrafn Traustason, Jennifer E. S. Szymanowski, Sara Mana, Peter C. Burns, Haylie L. Lobeck, Patrick A. Julien, John R FitzPatrick |
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Rok vydání: | 2019 |
Předmět: |
Aqueous solution
010405 organic chemistry Inorganic chemistry chemistry.chemical_element Uranium 010402 general chemistry 01 natural sciences Hydrothermal circulation Oxalate 0104 chemical sciences Inorganic Chemistry chemistry.chemical_compound Uranyl peroxide chemistry Phase (matter) Cage Nanoscopic scale |
Zdroj: | Dalton Transactions. 48:7755-7765 |
ISSN: | 1477-9234 1477-9226 |
DOI: | 10.1039/c9dt01529a |
Popis: | 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. |
Databáze: | OpenAIRE |
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