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Supercritical fluid deposition of Ru nanoparticles onto SiO2 SBA-15 as a sustainable method to prepare selective hydrogenation catalysts

机译:将Ru纳米颗粒超临界流体沉积在SiO2 SBA-15上作为制备选择性加氢催化剂的可持续方法

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Ru nanoparticles were successfully deposited onto mesoporous SiO2 SBA-15 using supercritical CO2 (scCO(2)). The use of scCO(2) favoured the metal dispersion and Ru nanoparticles uniformly distributed throughout the support were obtained. Different precursors and methodologies were employed: impregnation with Ru(tmhd)(2)(COD) in scCO(2) at 80 degrees C and 13.5 and 19.3 MPa and further reduction in H-2/N-2 at 400 degrees C at low pressure, reactive deposition of Ru(tmhd)(2)(COD) with H-2 in scCO(2) at 150 degrees C and reactive deposition of RuCl3 center dot xH(2)O with ethanol in scCO(2) at 150 and 200 degrees C. The size of the particles was limited in one dimension by the pore size of the support. The metal loading varied with the methodology and experimental conditions from 0.9 to 7.4% Ru mol. These materials exhibited remarkable catalytic activity. The Ru/SiO2 SBA-15 materials prepared by reactive deposition with H-2 in scCO(2) were selective catalysts for the hydrogenation reactions of benzene and limonene, allowing the production of partly hydrogenated hydrocarbons that may serve as building blocks for more complex chemicals. scCO(2) is shown to be a green solvent that allows the preparation of efficient heterogeneous catalysts to design sustainable processes. Furthermore, in the hydrogenation of limonene, scCO(2) was also used as the solvent.
机译:Ru纳米粒子已成功沉积到使用超临界CO2(scCO(2))的介孔SiO2 SBA-15上。使用scCO(2)有利于金属分散,并获得了均匀分布在整个载体中的Ru纳米粒子。使用了不同的前体和方法:在80°C和13.5 MPa和19.3 MPa的scCO(2)中用Ru(tmhd)(2)(COD)浸渍,并在400°C的低温下进一步还原H-2 / N-2压力,150°C下在scCO(2)中与H-2的Ru(tmhd)(2)(COD)与H-2的反应性沉积和150°C在scCO(2)中与乙醇的RuCl3中心点xH(2)O的反应性沉积200℃。颗粒的尺寸在一维上受到载体的孔径的限制。金属负载量随方法和实验条件从0.9%到7.4%Ru mol变化。这些材料表现出显着的催化活性。通过在scCO(2)中与H-2反应沉积制备的Ru / SiO2 SBA-15材料是苯和柠檬烯加氢反应的选择性催化剂,允许生产部分氢化的烃,可以作为更复杂化学物质的基础。 scCO(2)被证明是一种绿色溶剂,可以制备高效的多相催化剂来设计可持续的工艺。此外,在柠檬烯的氢化中,scCO(2)也用作溶剂。

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