Dataset of Supported Uranyl Photocatalyst on Hafnium-Metal-organic Layers for Alkylation of Cyclic Alcohols

Visible-light excitation of uranyl cations produces highly oxidizing excited states capable of activating inert chemical bonds. The process utilizes 238U-depleted uranium, a fission fuel byproduct enriched in 238U, 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.