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- Title
Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation.
- Authors
Ma, Mingwei; Chen, Enpeng; Yue, Huijuan; Tian, Ge; Feng, Shouhua
- Abstract
High-entropy metal-organic frameworks (HE-MOFs) hold promise as versatile materials, yet current rare examples are confined to low-valence elements in the fourth period, constraining their design and optimization for diverse applications. Here, a novel high-entropy, defect-rich and small-sized (32 nm) UiO-66 (ZrHfCeSnTi HE-UiO-66) has been synthesized for the first time, leveraging increased configurational entropy to achieve high tolerance to doping with diverse metal ions. The lattice distortion of HE-UiO-66 induces high exposure of metal nodes to create coordination unsaturated metal sites with a concentration of 322.4 μmol/g, which increases the abundance of Lewis acid-base sites, thereby achieving a significant improvement in the performance of the catalytic transfer hydrogenation (CTH) reaction. Systematic investigation manifests that the special electronic structure of HE-UiO-66 enhances the interaction and bonding with substrate molecules and reduces the energy barrier of the hydrogen transfer process. Our approach offers a new strategy for constructing coordination unsaturated metal sites in MOFs. High-entropy metal-organic frameworks offer significant potential as versatile materials, but existing examples are largely limited to low-valence elements in the fourth period, restricting their design and optimization for various applications. Here, a novel high-entropy, defect-rich, and small-sized UiO-66 framework has been synthesized to enhance catalytic transfer hydrogenation.
- Subjects
CATALYTIC hydrogenation; INORGANIC chemistry; ACTIVATION energy; METAL-organic frameworks; ELECTRONIC structure
- Publication
Nature Communications, 2025, Vol 16, Issue 1, p1
- ISSN
2041-1723
- Publication type
Academic Journal
- DOI
10.1038/s41467-024-52225-5