Ru/SiC催化乙酰丙酸水相加氢制备γ-戊内酯
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太原理工大学

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Efficient hydrogenation of levulinic acid to γ-valerolactone over Ru/SiC catalyst in aqueous
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Taiyuan University of Technology

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    摘要:

    为提高水相体系中催化乙酰丙酸(LA)加氢合成γ-戊内酯(GVL)催化剂的水热稳定性和耐酸稳定性,采用浸渍还原法制备Ru负载量为3%(以SiC质量为基准的质量分数)的Ru/SiC催化剂(Ru3/SiC),采用TEM、XRD、XPS、H2-TPR和H2-TPD对结构形貌、表面作用进行表征。将Ru3/SiC用于催化LA加氢反应,对比不同载体(石墨烯、TiO2,ZrO2、SiO2、Al2O3)制备的Ru负载催化剂(Ru3/石墨烯、Ru3/TiO2、Ru3/ZrO2、Ru3/SiO2和Ru3/Al2O3)与Ru3/SiC的催化性能,考察反应条件(反应温度、时间、氢气压力、溶剂)对Ru3/SiC催化LA加氢反应的影响和循环稳定性。结果表明,Ru3/SiC中的Ru纳米粒子(0.22 nm)主要以Ru0的形式均匀分散在SiC表面。与其他载体负载的Ru基催化剂相比,Ru3/SiC表现出更高的催化LA加氢反应活性,以LA(4 mmol)为反应物,水(10 mL)为溶剂,50 mg的Ru3/SiC为催化剂,H2压力0.2 MPa,反应温度50 ℃,反应时间2 h的条件下,LA转化率和GVL选择性均接近100%。Ru3/SiC循环5次后,活性无明显下降。Ru3/SiC的高催化活性主要是由于Ru与SiC之间的Mott-Schottky接触促进了载体与金属之间的电子转移,富电子的Ru纳米颗粒有利于H2的解离,从而提高了催化LA加氢反应的催化活性。

    Abstract:

    In order to improve the hydrothermal stability and acid resistance of the catalyst for the hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) in aqueous system, the Ru/SiC catalyst (Ru3/SiC) with a Ru loading capacity of 3% (mass fraction based on SiC mass) was prepared by a sample impregnation-reduction process. TEM, XRD, XPS, H2-TPR and H2-TPD were used to characterize the structure and surface effects of the catalysts. The catalytic performances of Ru catalysts with different support ( SiC, graphene, TiO2,ZrO2、SiO2、Al2O3) for the hydrogenation of LA were investigated. The influences of reaction conditions (reaction temperature, time, hydrogen pressure and solvent) on the hydrogenation of LA catalyzed by Ru3/SiC were studied. The results show that Ru nanoparticles (0.22 nm) in Ru3/SiC are mainly dispersed uniformly on the SiC surface in the form of Ru0. Compared with other supported Ru-based catalysts, Ru3/SiC showed higher catalytic activity for LA hydrogenation in water under mild conditions of 50 ℃, 0.2 MPa H2 for 2 h, and LA conversion rate and GVL selectivity are close to 100%. Moreover, Ru3/SiC activity did not decrease significantly after 5 cycles. The high catalytic activity of Ru3/SiC is due to the electron transfer through Mott-Schottky junction between Ru and SiC. The electron-rich Ru nanoparticles are favorable for H2 dissociation, thus enhancing the catalytic activity for hydrogenation reaction of LA.

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王静茹. Ru/SiC催化乙酰丙酸水相加氢制备γ-戊内酯[J].精细化工,2025,42(7):

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  • 收稿日期:2024-07-04
  • 最后修改日期:2024-08-09
  • 录用日期:2024-07-29
  • 在线发布日期: 2025-07-10
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