Self-assembly mechanism of Uranyl nanocapsules has been known for almost a decade. Crystals of monomers and POM capsules have been isolated and well characterized in both solution and solid state by techniques such as X-ray diffraction, X-ray scattering, multi-nuclear NMR, and vibrational spectroscopies. However, further details for the process of capsule self-assembly and to control the capsule geometry, size and monospecificity remains to be elucidated. We are currently investigating this reaction pathway, using as a model system, self-assembly of the [UO2(O2)OH]2424- (U24) capsule from the lithium monomer using Raman spectroscopy and Small-angle X-ray Scattering (SAXS). The surprising finding of this study is that we can completely turn this reaction on and off by the presence or absence of a catalyst that serves to decompose the peroxide ligand. While prior calorimetric studies indicated thermodynamic stability of the monomer compared to the capsules, the kinetics of the reaction has not been addressed. This current study suggests that there is indeed an energetic barrier to conversion of the monomer to the nanocapsule.

Catalysis: Uranyl monomer to U<sub>24</sub> nanocapsule

248th National Meeting (2014)

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Catalysis: Uranyl monomer to U24 nanocapsule

Catalysis: Uranyl monomer to U₂₄ nanocapsule