Synergistic Enhancement of Catalytic Activity in USY Zeolites Via Selective Aluminum Removal and Cerium Doping for Aniline Condensation
摘要
This study proposes a novel strategy to enhance the catalytic performance of USY zeolites through selective aluminum extraction using tartaric acid and cerium substitution, with a focus on their application in the condensation of aniline with diphenylamine. A comprehensive characterization approach encompassing XRD, BET, and SEM analysis revealed that treatment with 0.1 mol/L tartaric acid led to the effective removal of aluminum atoms from the zeolite framework, concurrently generating new micropores. This process resulted in a substantial enhancement in the accessibility of the reactants. Infrared spectroscopy of pyridine confirmed that the addition of 5% cerium compensated for the loss of aluminum by supporting the lattice and modulating the acid strength distribution. The optimized 0.1TA-5% Ce-USY catalyst achieved 14.3% aniline conversion at 320 °C, outperforming the majority of reported catalysts under comparable conditions. The combined modification produced a synergistic effect: the acid treatment created additional diffusion channels, while cerium doping stabilized the acid sites. This dual strategy not only maintained the structural integrity of the zeolite (92% crystallinity as determined by XRD), but also opened up new avenues for the design of highly efficient acid catalysts. These findings offer a comprehensive approach for designing highly efficient acid catalysts by selective elemental modification, with a broad spectrum of potential applications.
Graphical Abstract