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<p>The widespread applications of metal-organic frameworks are severely restricted due to their limited active sites and insufficient thermal stability. This study focuses on high-stability rare earth metal-organic frameworks (RE-MOFs), employing advanced strategies of heteroatom doping and defect engineering to gain RE-Ni-BTC materials. The incorporation of Ni into RE-MOFs modifies the charge distribution and crystal structure stability, giving rise to atomic-scale defects that facilitate the formation of a defect-induced RE–O frustrated Lewis pair (FLP) alongside a unique Ni–O<sub>4</sub> coordination structure. Notably, Nd-Ni-BTC outperforms Ce-Ni-BTC due to the enhanced Lewis acid-base properties and excellent adsorption/desorption of substrate molecules, enabling complete dicyclopentadiene (DCPD) conversion and at least seven cycles of recycling under conditions of 100 °C, 2 MPa, and 10 h. Therefore, this approach balances catalytic activity and stability without structural damage, opening a new route for defective MOFs in hydrogenation catalysis and future catalyst design.</p>

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Nickel-mediated formation of stable frustrated Lewis pairs in rare earth MOFs for dicyclopentadiene hydrogenation

  • 期刊论文

  • 发表日期：

    2025年5月9日

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  • Danfeng Zhao,
  • Jing Lin,
  • Rushuo Li,
  • Xinmeng Xu,
  • Fajie Hu,
  • Zhaokun Wang,
  • Xiubing Huang,
  • Ge Wang

摘要

The widespread applications of metal-organic frameworks are severely restricted due to their limited active sites and insufficient thermal stability. This study focuses on high-stability rare earth metal-organic frameworks (RE-MOFs), employing advanced strategies of heteroatom doping and defect engineering to gain RE-Ni-BTC materials. The incorporation of Ni into RE-MOFs modifies the charge distribution and crystal structure stability, giving rise to atomic-scale defects that facilitate the formation of a defect-induced RE–O frustrated Lewis pair (FLP) alongside a unique Ni–O4 coordination structure. Notably, Nd-Ni-BTC outperforms Ce-Ni-BTC due to the enhanced Lewis acid-base properties and excellent adsorption/desorption of substrate molecules, enabling complete dicyclopentadiene (DCPD) conversion and at least seven cycles of recycling under conditions of 100 °C, 2 MPa, and 10 h. Therefore, this approach balances catalytic activity and stability without structural damage, opening a new route for defective MOFs in hydrogenation catalysis and future catalyst design.