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

Lobeck, Haylie; Traustason, Hrafn; Julien, Patrick; Fitzpatrick, John; Mana, Sara; Szymanowski, Jennifer; Burns, Peter C.

doi:10.1039/C9DT01529A

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

Journal Article · Tue Jan 01 00:00:00 EST 2019 · Dalton Transactions

DOI:https://doi.org/10.1039/C9DT01529A· OSTI ID:1510719

Lobeck, Haylie ^[1]; Traustason, Hrafn ^[1]; Julien, Patrick ^[2]; Fitzpatrick, John ^[1]; Mana, Sara ^[3]; Szymanowski, Jennifer ^[1]; Burns, Peter C. ^[1]

Univ. of Notre Dame, Notre Dame, IN (United States)
McGill Univ., Montreal, QC (Canada)
Salem State Univ., Salem, MA (United States)

Aqueous solutions containing the nanoscale uranyl peroxide cage clusters U₆₀, [(UO₂)(O₂)(OH)]₆₀^60-, 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)]₂₄^24-, 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.

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

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003763

OSTI ID:: 1510719

Alternate ID(s):: OSTI ID: 1511506

Journal Information:: Dalton Transactions, Vol. 48, Issue 22; ISSN 1477-9226

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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