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Defect Engineering and Ni Promoter Synergize Electron Transfer to Ru⁰/UiO-66(Ce) for Mild DCPD Hydrogenation
Summary:
The authors from the University of Science and Technology Beijing developed a defective UiO-66(Ce) material with highly dispersed RuNi nanoparticles (Ru1Ni1.5@UiO-66(Ce)-12 h) for dicyclopentadiene hydrogenation, achieving 100% conversion and selectivity under mild conditions.
Background:
1. Olefin hydrogenation is crucial for industrial applications, but traditional methods often require harsh conditions such as high temperature and pressure, leading to energy consumption and low selectivity. Previous research has explored non-precious metal catalysts and noble metal catalysts, but they face challenges in mild reaction conditions and high costs.
2. The authors proposed a selective catalysis strategy using defective UiO-66(Ce) and a Ni promoter to enhance electron transfer to Ru0 sites, achieving high activity and selectivity under mild conditions.
Research Content:
1. Synthesis:
The authors synthesized defective UiO-66(Ce) using cyanuric acid as a molecular etching agent and further prepared Ru1Ni1.5@UiO-66(Ce)-12 h via a solution impregnation reduction method.
2. Characterizations:
1) BET analysis showed a specific surface area of 127.88 m²g⁻¹ and a pore size distribution with a peak at 1.3 nm.
2) SEM/TEM tests revealed a uniform distribution of C, N, O, Ru, and Ni elements, with a particle size of approximately 1 nm.
3) XPS and XAFS confirmed the formation of Ce-O-Ru/Ni heterointerfaces and electron transfer from Ni species to Ru species.
3. Application:
The material achieved 100% conversion of dicyclopentadiene to tetrahydrodicyclopentadiene with ~100% selectivity under mild conditions (35 °C, 1 MPa) in 25 minutes.
4. Mechanism:
The Ce-O-Ru/Ni heterointerfaces and Ni promoter synergistically enhanced electron transfer to Ru0 sites, promoting the adsorption and activation of H–H and C=C bonds, thus accelerating the hydrogenation process.
Outlook:
This research provides a promising strategy for designing noble metal-based catalysts with high activity and selectivity under mild conditions, offering valuable insights for the development of efficient olefin hydrogenation catalysts.
Defect engineering and Ni promoter synergistically accelerating electron transfer to Ru0 sites in UiO-66(Ce) for dicyclopentadiene hydrogenation under mild condition
Authors: Rushuo Li, Tao Ban, Danfeng Zhao, Jing Lin, Zhiyuan Liu, Linmeng Wang, Xiubing Huang, Zhiping Tao, Ge Wang
DOI: 10.1007/s12274-024-6954-1
Link: https://doi.org/10.1007/s12274-024-6954-1
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