Al-Doped Core-Shell-Structured Ni@Mesoporous Silica for Highly Selective Hydrodeoxygenation of Lignin-Derived Aldehydes

Selective deoxygenation of chemicals using non-noblemetal-basedcatalysts poses a significant challenge toward upgrading biomass-derivedoxygenates into advanced fuels and fine chemicals. Herein, we reporta bifunctional core-shell catalyst (Ni@Al-3-mSiO(2)) consisting of Ni nanoparticles closely encapsulated by theAl-doped mesoporous silica shell that achieves 100% vanillin conversionand >99% yield of 2-methoxy-4-methylphenol under 1 MPa H-2 at 130 & DEG;C in water. Due to the unique mesoporous core-shellstructure, no significant decrease in catalytic activity was observedafter 10 recycles. Furthermore, incorporating Al atoms into the silicashell significantly increased the number of acidic sites. Densityfunctional theory calculations reveal the reaction pathway of thevanillin hydrodeoxygenation process and uncover the intrinsic influenceof the Al sites. This work not only provides an efficient and cost-effectivebifunctional hydrodeoxygenation catalyst but also offers a new syntheticprotocol to rationally design promising non-noble metal catalystsfor biomass valorization or other widespread applications.