Core-shell meso-beta@mesoporous aluminosilicate supported Ni2P catalyst for the hydrodenitrogenation of quinoline: Effect of core shell structure on Ni2P particle size

Abstract

A core–shell structured material with a mesoporous aluminosilicate (MAS) shell and mesopore-containing beta zeolite (meso-beta) core was synthesized by self-assembly using triblock copolymer (P123) as template. The corresponding Ni2P catalyst for quinoline hydrodenitrogenation (HDN) was prepared by the hypophosphite disproportionation method. The core–shell support exhibits a wide pore structure, large surface area, suitable amounts of Lewis and Bronsted acid sites, and a large number of acidic hydroxyl groups exist at the interface of MAS and meso-beta. These properties contribute to the formation of very small (4.7 nm) Ni2P clusters. Furthermore, the micropores of the zeolite core can anchor the Ni2P nanoparticles and prevent nanoparticle aggregation. The smaller Ni2P particle size can expose more active sites and thus results in higher catalytic activity. The obtained Ni2P/meso-beta@MAS catalyst exhibits a higher reaction rate constant and TOF (12.37 × 10-2 μmolg−1s−1 and 1.7 × 10−3s−1, respectively) for the quinoline HDN reaction compared to a silica-supported Ni2P catalyst (6.18 × 10−2 μmolg−1s−1 and 1.5 × 10−3s−1, respectively) and Ni2P/H-beta catalyst (6.81 × 10−2 μmolg−1s−1 and 1.4 × 10−3s−1, respectively).