Hydrodeoxygenation of Lignin and Its Derivatives Using a Ruthenium Supported on the Sintered Black Carbon and Metal-Organic Framework
摘要
Conventional fossil fuels represent non-renewable energy resources that contribute significantly to environmental pollution, primarily through the emission of black carbon (BC). Given the urgent need to develop sustainable energy alternatives and utilize waste resources, this study reports the synthesis of a defective yet stable sponge-like catalyst through the anchoring of ruthenium (Ru) nanoparticles on a hybrid substrate composed of BC and carbonized Metal-Organic Framework-303 (MOF-303). Systematic optimization of the BC/MOF-303 mass ratio and sintering temperature yielded a catalyst exhibiting exceptional performance in the heterogeneous phase hydrodeoxygenation (HDO) of vanillin (VAN) to 2-methoxy-4-methylphenol (MMP) under mild conditions (1 MPa H2, 220 °C, 1.5 h). The optimized catalyst achieved complete VAN conversion with an MMP selectivity of 92%. Furthermore, the catalyst demonstrated remarkable reusability, maintaining high activity over five consecutive reaction cycles, and exhibited broad applicability to various lignin-derived compounds as well as raw lignin. Structural characterization revealed that the integration of BC and MOF-303 formed a defective substrate characterized by a well-developed porous architecture and abundant active sites. Notably, the nitrogen-containing moieties within MOF-303 facilitated the formation of Ru-N chelates, which enhanced the adsorption and polarization of C = O bonds, thereby promoting the HDO reaction pathway. This work not only provides a viable strategy for designing sustainable and efficient lignin conversion catalysts but also advances the valorization of industrial waste materials.
Graphical Abstract