Fabrication of highly dispersed Ru nanoparticles stabilized in coated carbon shell via one-pot co-synthesis strategy for aqueous hydrogenation of bio-based itaconic acid

摘要

Metal nanoparticles catalysts are widely used in hydrogenation of carboxylic acids and their derivatives, which are significant reactions to produce high-value compounds such as alcohols and lactones. These reactions were usually carried out in liquid phase at harsh conditions with high temperature and pressure, however, catalysts deactivation frequently occurred since small metal NPs were inclined to migrate and aggregate as well as dissolve and leach in such acid systems. Thus, it's a great challenge to prepare catalysts with highly dispersed small metal NPs with good stability and durability. Herein we propose a novel one-pot co-synthesis method to prepare highly dispersed and stabilized nanometal catalysts that small Ru NPs embedded in carbon species coated on silica nanospheres. Ru precursors were doped directly in the synthesis of RF coated silica spheres along with the polymerization of resorcinol-formaldehyde, and following the process of carbothermal reduction. Aqueous hydrogenation of itaconic acid was used as a probe reaction, which could produce high-value products such as methylsuccinic acid and methyl butyrolactone. The as-prepared catalysts had uniform dispersion of small Ru NPs with core-shell structure of resin coated silica nanospheres, exhibited good hydrogenation activity and stability with no obvious loss of yield for methyl butyrolactone and less sintering in recycling tests.