Abstract
Hydrogenation of levulinic acid (LA) obtained from cellulose biomass is a promising path for production of γ-valerolactone (GVL)—a component of biofuel. In this work, we developed Ru nanoparticle containing nanocomposites based on hyperbranched pyridylphenylene polymer, serving as multiligand and stabilizing matrix. The functionalization of the nanocomposite with sulfuric acid significantly enhances the activity of the catalyst in the selective hydrogenation of LA to GVL and allows the reaction to proceed under mild reaction conditions (100 °C, 2 MPa of H2) in water and low catalyst loading (0.016 mol.%) with a quantitative yield of GVL and selectivity up to 100%. The catalysts were successfully reused four times without a significant loss of activity. A comprehensive physicochemical characterization of the catalysts allowed us to assess structure-property relationships and to uncover an important role of the polymeric support in the efficient GVL synthesis.
Highlights
Levulinic acid (LA) is one of the substances that can be obtained from cellulosic biomass via acid hydrolysis [1]
Ru NPs were obtained by thermal decomposition of Ru(acac)3 in the reaction solution of pre-synthesized hyperbranched pyridylphenylene polymers (PPP) [37] in benzyl ether at 285 ◦ C in argon, giving the catalyst notated as Ru(acac)3 in the presence of PPP (Ru-PPP) (Figure 1)
As the levulinic acid (LA) hydrogenation is facilitated in the presence of acidic sites located in close proximity to the Ru species [22,32], we introduced acidic groups in Ru-PPP by a brief treatment with sulfuric acid (95–98%) at room temperature
Summary
Levulinic acid (LA) is one of the substances that can be obtained from cellulosic biomass via acid hydrolysis [1]. It is an important compound in biofuel production because it serves as a universal building block for syntheses of liquid fuel components [2]. LA hydrogenation to GVL is a catalytic process in which both homogeneous [6] and heterogeneous [7,8] catalysts are used. Despite the high activity of homogeneous catalysts, the application of supported metal catalysts in industrial processes is especially beneficial due to ease of product recovery and the possibility of catalyst reuse
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