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Solid-State Dynamics of Uranyl Polyoxometalates

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https://ir.library.oregonstate.edu/concern/articles/rb68xd718

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  • Understanding fundamental uranyl polyoxometalate (POM) chemistry in solution and the solid state is the first step to defining its future role in the development of new actinide materials and separation processes that are vital to every step of the nuclear fuel cycle. Many solid-state geometries of uranyl POMs have been described, but we are only beginning to understand their chemical behavior, which thus far includes the role of templates in their self-assembly, and the dynamics of encapsulated species in solution. This study provides unprecedented detail into the exchange dynamics of the encapsulated species in the solid state through Magic Angle Spinning Nuclear Magnetic Resonance (MAS NMR) spectroscopy. Although it was previously recognized that capsule-like molybdate and uranyl POMs exchange encapsulated species when dissolved in water, analogous exchange in the solid state has not been documented, or even considered. Here, we observe the extremely high rate of transport of Li⁺ and aqua species across the uranyl shell in the solid state, a process that is affected by both temperature and pore blocking by larger species. These results highlight the untapped potential of emergent f-block element materials and vesicle-like POMs.
  • Keywords: polyoxometalate, solid-state NMR, uranyl, proton MAS NMR, ion-exchange
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  • Alam, T. M., Liao, Z., Zakharov, L. N. and Nyman, M. (2014). Solid-State Dynamics of Uranyl Polyoxometalates. Chemistry: A European Journal, 20: 8302–8307. doi:10.1002/chem.201402351
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  • 20
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  • 27
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  • This work was supported as part of the Materials Science of Actinides, an Energy Frontier Research Center funded by the Department of Energy, Office of Science, Office of Basic Energy Sciences under award number DE-SC0001089. The NMR component of the work (T.M.A.) was performed at Sandia National Laboratories, which is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin company, for the U. S. Department of Energy’s National Nuclear Security Administration under contract DE-AC04–94AL85000.
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