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Title: Solid-State Transformation of Uranyl Peroxide Materials through High-Level Irradiation

Journal Article · · Inorganic Chemistry
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]
  1. University of Notre Dame, IN (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); University of Notre Dame
  2. University of Notre Dame, IN (United States)
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The solid-state transformation of sodium uranyl triperoxide (Na4(UO2)(O2)3·9H2O, NaUT) to sodium uranyl tricarbonate (Na4(UO2)(CO3)3) by radiolysis was observed for the first time. The exposure of NaUT to 3 MGy gamma irradiation resulted in partial breakdown of the peroxides forming a mixed peroxide and carbonate species. The effects of He-ion irradiation on NaUT were also investigated up to 225 MGy using both hydrated argon and dry argon. The complete conversion to the uranyl tricarbonate phase by 56 MGy was done using hydrated argon, while dry argon did not fully convert showing the importance of water in the system. He-ion irradiated NaUT samples all convert to the tricarbonate phase with time in air post radiation exposure. This transition was monitored via Raman spectroscopy, infrared spectroscopy (IR), and powder X-ray diffraction (PXRD) to further confirm the identity of the final product as the sodium uranyl tricarbonate, čejkaite. Furthermore, this transformation outlines a mechanism for the mobility of uranyl in natural environments and in the Hanford tanks.

Research Organization:
University of Notre Dame, IN (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
NA0003763; 89233218CNA000001
OSTI ID:
2221776
Alternate ID(s):
OSTI ID: 2426819
Journal Information:
Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 48 Vol. 62; ISSN 0020-1669
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
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