Exploring the Structure and Photophysical Properties of Actinide Hybrid Materials Utilizing Viologen Cations
Open Access DepositedThe photophysical properties of actinyl-bearing materials are indicative offundamental characteristics that govern their reactivity and chemical behavior, which are crucial aspects of nuclear waste stewardship and forensics. Herein we probe the photoreactivity of such materials and elucidate the role of assembly and non-covalent interactions on their behavior. We do this through the systematic pairing of actinyl anions with 1,1’-disubstituted-4,4’-bipyridinium cations, i.e. viologens, species known for their ability to induce radicalization upon exposure to light. When paired with the uranyl anion, this approach consistently produces materials that exhibit photoreactivity in the form progressive quenching of characteristic luminescent emission. This behavior is indicative of photoinduced electron transfer from the uranyl anion to the viologen cation (as evidenced by EPR spectroscopy). We use this template to probe structure-property relationships of photoreactivity by engineering assembly with halogenated viologens and measuring reactivity across uranyl species. Additionally, we utilize this straightforward synthetic methodology to produce novel transuranic-viologen material so we may probe similar behavior across the 5f-block and investigate the role of f-electrons in photophysical behavior. This work resulted in the synthesis of 22 novel actinide-viologen hybrid materials and the elucidation of the role of assembly and composition on photoreactivity.
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