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Supported Uranyl Photocatalyst on Hafnium-Metal-organic Layers for Alkylation of Cyclic Alcohols
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DOI：10.1039/D5CY00840A.png)
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Abstract
En 中文
Visible-light excitation of uranyl cations produces highly oxidizing excited states capable of activating inert chemical bonds. The process utilizes 238 U-depleted uranium; a fission fuel byproduct enriched in 238 U; which has significantly lower radioactivity and is safe for practical use. However; homogeneous uranyl photocatalysis suffers from limited recyclability and potential uranium contamination concerns even with low radioactivity. Therefore; immobilization of depleted uranyl onto suitable supports is critical. To address these limitations; we implemented two distinct post-synthetic modification strategies targeting the secondary building units (SBUs) and organic linkers separately; enabling effective immobilization of uranyl ions on hafnium-based metal-organic layers (BTB/TPY-Hf-MOLs). Characterization revealed that BTB-Hf-MOL-U forms surface-bound uranyl species predominantly in the form of uranium oxide (UO3) nanoparticles; while TPY-Hf-MOL-U generates a single-site heterogeneous catalyst through ligand chelation. Under blue LED irradiation; BTB-Hf-MOL-U demonstrates noteworthy catalytic efficiency and diastereoselectivity; whereas TPY-Hf-MOL-U exhibited superior cycling stability.
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