Nature Chemistry
Nature Chemistry
5 years ago

Elucidating bonding preferences in tetrakis(imido)uranate(VI) dianions

Elucidating bonding preferences in tetrakis(imido)uranate(VI) dianions
Matthias Zeller, Debmalya Ray, Suzanne C. Bart, Nickolas H. Anderson, Laura Gagliardi, Jing Xie
Actinyl species, [AnO2]2+, are well-known derivatives of the f-block because of their natural occurrence and essential roles in the nuclear fuel cycle. Along with their nitrogen analogues, [An(NR)2]2+, actinyls are characterized by their two strong trans-An–element multiple bonds, a consequence of the inverse trans influence. We report that these robust bonds can be weakened significantly by increasing the number of multiple bonds to uranium, as demonstrated by a family of uranium(VI) dianions bearing four U–N multiple bonds, [M]2[U(NR)4] (M = Li, Na, K, Rb, Cs). Their geometry is dictated by cation coordination and sterics rather than by electronic factors. Multiple bond weakening by the addition of strong π donors has the potential for applications in the processing of high-valent actinyls, commonly found in environmental pollutants and spent nuclear fuels.

Publisher URL: http://dx.doi.org/10.1038/nchem.2767

DOI: 10.1038/nchem.2767

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