Single-Crystal Time-of-Flight Neutron Diffraction and Magic-Angle-Spinning NMR Spectroscopy Resolve the Structure and ¹H and ⁷Li Dynamics of the Uranyl Peroxide Nanocluster U₆₀

Single-crystal time-of-flight neutron diffraction has provided atomic resolution of H atoms of H₂O molecules and hydroxyl groups, as well as Li cations in the uranyl peroxide nanocluster U₆₀. Solid-state magic-angle-spinning nuclear magnetic resonance (MAS NMR) spectroscopy was used to confirm the dynamics of these constituents, revealing the transportation of Li atoms and H₂O through cluster walls. H atoms of hydroxyl units that are located on the cluster surface are involved in the transfer of H₂O and Li cations from inside to outside and vice versa. This exchange occurs as a concerted motion and happens rapidly even in the solid state. As a consequence of its large size and open hexagonal pores, U₆₀ exchanges Li cations more rapidly compared to other uranyl nanoclusters.