Compared to other parts of the periodic table, relatively little is known about the role of 5f electrons in bonding and the impact of orbital overlap between the 5f, 6d, and 7s orbitals in actinides. Studies of actinide materials in extreme conditions such as high pressure probe the complex bonding of the actinides. Uranium is of particular interest due to its prevalence in nuclear energy and nonproliferation programs. The goal of this project is to further elucidate the nature of U(VI) bonding through pressure-induced structural changes in uranyl compounds relevant to nuclear waste and mineralogical environments. High (gigapascal (GPa) range) pressures were achieved experimentally using a diamond anvil cell (DAC). Raman spectroscopy and X-ray diffraction were used to probe the short- and long-range structure of materials, respectively, at high pressures. Preliminary results indicate reversible pressure-induced bond shortening and sheet compression in boltwoodite (K,Na[(UO2)(SiO3OH)]1.5H2O).

High pressure studies of uranyl compounds to enhance understanding of 5f-orbital bonding

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ACS Fall 2022

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