Emory Zoe C, LaVerne Jay A, Burns Peter C
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, USA.
Radiation Laboratory, University of Notre Dame, Notre Dame, Indiana 46556, USA.
Dalton Trans. 2024 Oct 29;53(42):17169-17178. doi: 10.1039/d4dt01841a.
The solid form of the uranyl peroxide cage (UPC) cluster LiU (Li[(UO)(O)]) was irradiated by 5 MeV He ions to achieve doses up to 42 MGy. An intermediate compound formed that reacts with atmospheric CO 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 He 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-U salts before and after He irradiation. The highest yield of uranyl carbonates occurred when hydrated Ar gas was flowed across the sample during He irradiation. Electron paramagnetic resonance spectroscopy provided evidence of hydroxyl and superoxide radicals in both unirradiated and γ-irradiated Li-U.
用5兆电子伏特的氦离子辐照过氧化铀酰笼状（UPC）簇合物LiU（Li[(UO)(O)]）的固体形式，剂量高达42兆戈瑞。形成了一种中间化合物，它与大气中的CO反应生成碳酸铀酰。通过在氦离子辐照期间让干燥或含水的氩气在样品上流动，以及在辐照前后将样品储存在干燥和潮湿环境中，研究了水在UPC向碳酸铀酰转化过程中的作用。利用拉曼光谱、红外光谱、X射线光电子能谱和电喷雾电离质谱对氦离子辐照前后的固体Li-U盐进行了表征。当在氦离子辐照期间让含水的氩气流过样品时，碳酸铀酰的产率最高。电子顺磁共振光谱提供了未辐照和γ辐照的Li-U中羟基和超氧自由基的证据。
