Actinides have fascinating chemical properties due to the complex nature of their 5f electrons that may lead to unique catalytic, electronic, and optical properties.  Of particular interest is the development of novel actinide complexes to improve advanced separations technologies, long-term storage of nulcear materials, and environmental remediation  We use a variety of low-temperature synthesis techniques to create novel materials containing uranium (²³⁸U), and neptunium (²³⁷Np) that are characterized by single-crystal X-ray diffraction, NMR, Raman and IR spectroscopy, and thermogravimetric analysis.  We are specifically focused on high valent actinides (+5 and +6) that form the actinyl cation because these states are most relevant to nuclear waste and environmental systems.  The actinyl cation contains the Np or U cation bonded to two oxygen atoms to create a nearly linear triatomic species.  Due to these strong bonds, the oxygen atoms are typically considered passivated, but they can become more reactive depending on the oxidation state of the actinide cation, the strength of intermolecular forces, presence of radical species, and light flux.  The Forbes research group focuses on understanding the reactivity of the actinyl oxo group under a range of conditions to develop means to control the chemical and physical properties of the actinide elements.