AI Article Synopsis
- - The research introduces new heterometallic frameworks containing transuranic elements, specifically the first instances of U/Pu-metal-organic frameworks (MOFs) and a unique monometallic Pu-analog.
- - The study examines the kinetics and thermodynamics involved in forming these actinide-MOFs and identifies a rate for U-to-Th transmetallation, suggesting uranyl species play a key role in solid-state reactions.
- - The findings highlight the stability and integration capacity of actinide materials, paving the way for advancements in applications like radioisotope thermoelectric generators and metalloradiopharmaceuticals.
Article Abstract
A novel series of heterometallic f-block-frameworks including the first examples of transuranic heterometallic U/ Pu-metal-organic frameworks (MOFs) and a novel monometallic Pu-analog are reported. In combination with theoretical calculations, we probed the kinetics and thermodynamics of heterometallic actinide(An)-MOF formation and reported the first value of a U-to-Th transmetallation rate. We concluded that formation of uranyl species could be a driving force for solid-state metathesis. Density of states near the Fermi edge, enthalpy of formation, band gap, proton affinity, and thermal/chemical stability were probed as a function of metal ratios. Furthermore, we achieved 97 % of the theoretical maximum capacity for An-integration. These studies shed light on fundamental aspects of actinide chemistry and also foreshadow avenues for the development of emerging classes of An-containing materials, including radioisotope thermoelectric generators or metalloradiopharmaceuticals.
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| http://dx.doi.org/10.1002/anie.202216349 | DOI Listing |
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