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Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation

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Listed:
  • Mingwei Ma

    (Jilin University)

  • Enpeng Chen

    (Jilin University)

  • Huijuan Yue

    (Jilin University)

  • Ge Tian

    (Jilin University)

  • Shouhua Feng

    (Jilin University)

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.

Suggested Citation

  • Mingwei Ma & Enpeng Chen & Huijuan Yue & Ge Tian & Shouhua Feng, 2025. "Entropy engineering activation of UiO-66 for boosting catalytic transfer hydrogenation," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-024-52225-5
    DOI: 10.1038/s41467-024-52225-5
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    References listed on IDEAS

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    1. Zhidong An & Piaoping Yang & Delong Duan & Jiang Li & Tong Wan & Yue Kong & Stavros Caratzoulas & Shuting Xiang & Jiaxing Liu & Lei Huang & Anatoly I. Frenkel & Yuan-Ye Jiang & Ran Long & Zhenxing Li , 2023. "Highly active, ultra-low loading single-atom iron catalysts for catalytic transfer hydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Xiang, Wenlong & Ren, Jie & Chen, Si & Shen, Chenyang & Chen, Yifei & Zhang, Minhua & Liu, Chang-jun, 2020. "The metal–organic framework UiO-66 with missing-linker defects: A highly active catalyst for carbon dioxide cycloaddition," Applied Energy, Elsevier, vol. 277(C).
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