Highly Stable and Selective Catalysts for m-Cresol Hydrogenolysis to Aromatics

Abstract

Deoxygenation is an essential link for upgrading bio-based low-value phenolics to aromatics, which is achieved through the catalytic hydrogenation way. Herein, we designed and synthesized kinds of Ni-confined catalysts via tailoring the preparation procedures. The highest hydroxyl hydrogenolysis performance (r[garomatics·gNi–1·h–1] = 103.5 at 290 °C) in vapor m-cresol conversion so far was obtained over Ni@Silicalite-1 prepared via the in situ encapsulation method due to the average 2.5 nm Ni nanoparticles uniformly encapsulated within silicalite-1 crystals for improving the shape selectivity with the vertical adsorption mode of phenolics. The appropriate porosities are proven to play a crucial role in shape-selective catalysis for hydroxyl hydrogenolysis of m-cresol. In addition, Ni@Silicalite-1 showed outstanding stability in 200 h long run with 95.5% conversion and 74.2% aromatics yield without obvious deactivation. This work provided a novel insight into tuning hydroxyl hydrogenolysis of phenolics by designing metal@zeolite catalysts with different microenvironments and ultrasmall metal nanoparticles.