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Bimetallic PtFe-Catalyzed Selective Hydrogenation of Furfural to Furfuryl Alcohol: Solvent Effect of Isopropanol and Hydrogen Activation

机译:Bimetallic PTFE催化的糠醛至糠醇的选择性氢化:异丙醇和氢活化的溶剂作用

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摘要

Highly selective liquid-phase hydrogenation of furfural was efficiently catalyzed by PtFe alloy nanoparticles supported on CeO2. An initial reaction rate at similar to 1500 h(-1), a near 100% selectivity toward furfuryl alcohol (FA), and a satisfactory recycling stability were achieved on Pt3Fe/CeO2 catalyst. Based on the well-established knowledge of the modification effects of Fe additives on the geometric and electronic properties of Pt sites, this work further demonstrated that the bimetallic PtFe sites could promote H-2-activated dissociation for accelerating the hydrogenation reaction in comparison with the monometallic Pt/CeO2 catalyst. The results of isotopic and kinetic experiments to study the solvent effects elucidated that the reaction pathway of catalytic transfer hydrogenation with isopropanol as the hydrogen donor could be ruled out. The results also suggested that isopropanol-involved hydrogen exchange processes with hydrogen and FA could easily occur during the reactions. Furthermore, the furfural hydrogenation could be significantly affected by the solvent intermolecular hydrogen bonding interactions.
机译:PTFE合金纳米颗粒在CeO2上得到高效地催化糠醛的高度选择性液相氢化。在PT3FE / CeO 2催化剂上实现了与1500h(-1)相似的初始反应速率,对糠醇(FA)的接近100%选择性,以及令人满意的再循环稳定性。基于对PT位点几何和电子性质的Fe添加剂的修饰效果的良好知识,这项工作进一步证明了双金属PTFE位点可以促进H-2-活化的解离,以加速氢化反应相比之下单金属Pt / CeO2催化剂。研究溶剂效果的同位素和动力学实验的结果阐明了催化转移氢化与异丙醇作为氢供体的反应途径可以排出。结果还表明,在反应期间,异丙醇涉及具有氢气和FA的氢气交换过程。此外,糠醛氢化可显着受溶剂分子间氢键相互作用的显着影响。

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