Regulation of Ni valence state and synergistic effects of supports in the hydrodeoxygenation of lignin-derived vanillin using pseudoboehmite-supported Ni catalysts

Preparing 2-methoxy-4-methylphenol (MMP) through the vanillin (VAN) route is a crucial step in the high-value utilization of lignin (VTM). In this study, a series of Ni/PB catalysts were synthesized using pseudoboehmite (PB) as a carrier. Changes in the valence states of Ni were induced through H₂ activation, while the impacts of reaction temperature, initial pressure, and catalyst addition were investigated based on the VTM process. The results revealed that PB exhibited a distinct mesoporous structure (average pore size of 5.8 nm), with Ni loaded in small particles size (3.88 nm). Ni species on the catalyst existed in a + 2-valence state, undergoing a change after H₂ activation, with an increase in Ni⁰ promoting enhanced activity. The Ni/PB-450 catalyst exhibited excellent activity at 250°C for 3 hours (VAN conversion and MMP selectivity > 99%), and the catalyst demonstrated good durability, maintaining 99.1% VAN conversion and 80% MMP selectivity after two cycles. Combining the characterization and experimental results, the etherification and hydrogenation of VAN were identified as the primary reaction pathways. This study aimed to provide a new avenue for the high-value utilization of lignin and its derivatives through controlled catalyst preparation.