Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation
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-si...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-52225-5 |
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| author | Mingwei Ma Enpeng Chen Huijuan Yue Ge Tian Shouhua Feng |
| author_facet | Mingwei Ma Enpeng Chen Huijuan Yue Ge Tian Shouhua Feng |
| author_sort | Mingwei Ma |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-885b47db1e0d4fc78891c0ffa8b2c213 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-885b47db1e0d4fc78891c0ffa8b2c2132025-01-05T12:37:33ZengNature PortfolioNature Communications2041-17232025-01-0116111210.1038/s41467-024-52225-5Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenationMingwei Ma0Enpeng Chen1Huijuan Yue2Ge Tian3Shouhua Feng4State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin UniversityAbstract 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.https://doi.org/10.1038/s41467-024-52225-5 |
| spellingShingle | Mingwei Ma Enpeng Chen Huijuan Yue Ge Tian Shouhua Feng Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation Nature Communications |
| title | Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation |
| title_full | Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation |
| title_fullStr | Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation |
| title_full_unstemmed | Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation |
| title_short | Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation |
| title_sort | entropy engineering activation of uio 66 for boosting catalytic transfer hydrogenation |
| url | https://doi.org/10.1038/s41467-024-52225-5 |
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