Synthesis and characterization of Pd/ZSM-5/MCM-48 biporous catalysts with superior activity for benzene oxidation

Abstract

ZSM-5/MCM-48 composite materials with different acidities and enhanced thermal stability have been synthesized via a simple and reliable in situ overgrowth method. The as-prepared biporous materials and the Pd-impregnated catalysts were systematically investigated by various techniques, including XRD, ICP-OES, N2 adsorption/desorption, H2 chemisorption, SEM, TEM/HRTEM, FT-IR, 27Al MAS NMR, NH3-TPD, H2-TPR and XPS. The characterization results reveal that all composite catalysts exhibit high surface area, large pore volume and long pore diameter. The quantity of acid sites increases as the ZSM-5 additive amount increases, and Al atoms are in the tetrahedral coordination positions in composite materials. The activity tests demonstrate that all the Pd-loaded catalysts are active in the total elimination of benzene, while the catalytic activity values of Pd-loaded ZSM-5/MCM-48 composite catalysts are much higher than those of Pd/ZSM-5 or Pd/MCM-48 alone. Both Pd0 and Pd2+ are responsible for the oxidation reaction, and the catalytic activities are primarily related to the support acidity and the Pd dispersion. In addition, the stability of the composite catalysts also improves with an appropriate amount of ZSM-5 additives in MCM-48. This research shows that the novel Pd-loaded composite catalysts are promising materials in the elimination of VOCs.