Activation of uranyl peroxides by ionizing radiation prior to uranyl carbonate formation†

IF 4.3 3区材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC ACS Applied Electronic Materials Pub Date : 2024-09-26 DOI:10.1039/D4DT01841A

Zoe C. Emory, Jay A. LaVerne and Peter C. Burns

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Abstract

The solid form of the uranyl peroxide cage (UPC) cluster LiU₂₈ (Li₂₈[(UO₂)₂₈(O₂)₄₂]) was irradiated by 5 MeV He²⁺ ions to achieve doses up to 42 MGy. An intermediate compound formed that reacts with atmospheric CO₂ to form uranyl carbonates. The role of water in the UPC to uranyl carbonate transformation was studied by flowing either dry or hydrated Ar over samples during He²⁺ irradiation, and by storing samples in dry and humid environments before and after irradiation. Raman, infrared, and X-ray photoelectron spectroscopies and electrospray ionization mass spectrometry were used to characterize solid Li–U₂₈ salts before and after He²⁺ irradiation. The highest yield of uranyl carbonates occurred when hydrated Ar gas was flowed across the sample during He²⁺ irradiation. Electron paramagnetic resonance spectroscopy provided evidence of hydroxyl and superoxide radicals in both unirradiated and γ-irradiated Li–U₂₈.

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碳酸铀形成前电离辐射对过氧化铀的活化作用

过氧化铀笼（UPC）簇 LiU28（Li28[(UO2)28(O2)42]）的固态形式受到 5 MeV He2+ 离子的辐照，剂量高达 42 MGy。形成的中间化合物与大气中的二氧化碳反应生成铀碳酸盐。通过在氦2+辐照期间将干燥或水合氩流过样品，以及在辐照前后将样品储存在干燥和潮湿的环境中，研究了水在铀化合碳酸铀转化过程中的作用。拉曼光谱、红外光谱和 X 射线光电子能谱以及电喷雾离子化质谱法被用来表征 He2+ 辐照前后的固体 Li-U28 盐。在 He2+ 辐照期间，当水合 Ar 气体流过样品时，铀碳酸盐的产量最高。电子顺磁共振光谱提供了未经辐照和 -irradiated Li-U28 中羟基和超氧自由基的证据。

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