Theoretical investigation of U(i) arene complexes: is the elusive monovalent oxidation state accessible?

2019 ◽  
Vol 43 (3) ◽  
pp. 1469-1477 ◽  
Author(s):  
Jia-Nan Tian ◽  
Ming Zheng ◽  
Li Li ◽  
Georg Schreckenbach ◽  
Yuan-Ru Guo ◽  
...  

With the goal to extend the uranium oxidation state, relativistic DFT unravels an energetically favored U(i) complex of a heterocalix[4]arene.

1991 ◽  
Vol 257 ◽  
Author(s):  
Catherine Chisholm-Brause ◽  
Steven D. Conradson ◽  
P. Gary Eller ◽  
David E. Morris

ABSTRACTThe speciation of UO22+ and UO22+/ TBP mixtures has been investigated in solution and intercalated with the reference smectite clay SAz-1 using x-ray absorption, Raman, andluminescence spectroscopies. Neither aquated UO22+ nor its TBP complex undergoes any detectable changes in uranium oxidation state on intercalation. Further, at the pH values employed in this work, there is no evidence for hydrolysis of the uranium species to generate dimeric or higher order uranium oligomers. However, we do find indications that the structures of the solution complexes are altered on intercalation, particularly for the UO22+TBP system and for more dilute UO22+/aqueous systems. In addition, several lines of evidence suggest that, at the loading levels used in this study, the uranyl species is interacting with two or more spectroscopically distinguishable sites on SAz-1.


2002 ◽  
Vol 189 (3-4) ◽  
pp. 213-230 ◽  
Author(s):  
David Soudry ◽  
Sarah Ehrlich ◽  
Olga Yoffe ◽  
Yaacov Nathan

2002 ◽  
Vol 713 ◽  
Author(s):  
Gini Curran ◽  
Yoann Sevestre ◽  
Wendy Rattray ◽  
Patrick G. Allen ◽  
Ken R. Czerwinski

ABSTRACTThoria-urania-zirconia ceramics were studied in order to investigate the long-term behavior of potential thorium fuels in a repository environment. The ceramics were prepared by coprecipitation of the metal salts. Zirconia was added to determine if further stabilization against dissolution of the thoria-urania system could be achieved. In addition, 0.5 wt% MgO was added to some samples to increase stability and density. The inclusion of Zr in the ceramics did not dramatically decrease the leaching of thorium from the matrix.Material properties of the ceramic were analyzed using electron microscopy techniques such as Energy Dispersive X-ray (EDX) analysis and Electron Energy Loss Spectroscopy (EELS). X-ray diffraction and synchrotron-based x-ray absorption studies including extended xray fine structure (EXAFS) and x-ray absorption near edge spectroscopy (XANES) were also used to reveal elements of the phase structure and chemistry of the ceramics. X-ray diffraction (XRD) and EDX show that these ceramics separate into a zirconium-based phase and an actinide-based phase with low mutual affinity of thorium and zirconium, as well as partial solubilization of uranium in zirconium. The comparison of EELS spectra collected for the ceramics with spectra collected for UO2 and U3O8 reference materials also allow the assessment of uranium oxidation state independently in the two separate phases. Assessment of the bulk oxidation state using XANES correlated well with the EELS analysis. Interatomic distances and the bulk crystal structure were determined using EXAFS.


2020 ◽  
Vol 62 (5) ◽  
pp. 608-616
Author(s):  
K. I. Maslakov ◽  
V. G. Yarzhemsky ◽  
Yu. A. Teterin ◽  
A. Yu. Teterin ◽  
K. E. Ivanov

2020 ◽  
Vol 385 ◽  
pp. 265-273
Author(s):  
Yu-Cheng Liu ◽  
Chen-Hao Yeh ◽  
Yen-Fan Lo ◽  
Santhanamoorthi Nachimuthu ◽  
Shawn D. Lin ◽  
...  

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