Preparation of Ni/(ZSM-5/SAPO-11) catalyst and catalytic hydroconversion of coal tar pitch
摘要
Transforming coal tar pitch (CTP) into cleaner fuels and high-value chemicals has attracted considerable attention, largely due to its intricate molecular architecture, high content of polycyclic aromatic hydrocarbons (PAHs), and the environmental concerns associated with its direct use. In this work, we designed a mesoporous zeolite Socony Mobil-5 (ZSM-5)/silicoaluminophosphate-11 (SAPO-11) via hydrothermal synthesis and subsequently introduced Ni nanoparticles (NNPs) using a deposition-precipitation technique, yielding Ni/(ZSM-5/SAPO-11) catalyst with a well-developed hierarchical pore system. Comprehensive structural analyses—employing X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), NH3 temperature-programmed desorption (NH3-TPD), pyridine infrared (Py-IR), and X-ray photoelectron spectroscopy (XPS)—revealed that the Ni was highly dispersed throughout the zeolitic framework. To probe catalytic performance under various conditions, anthracene was selected as a model compound. Remarkably, complete hydrogenation of anthracene was achieved after just 1 h of reaction in n-hexane at 160 °C under an initial hydrogen pressure (IHP) of 4 MPa, highlighting the catalyst’s exceptional activity under relatively mild catalytic hydroconversion (CHC) conditions. Furthermore, when applied to the extractable portion (EP) of CTP under the same temperature and pressure for 18 h, the catalyst facilitated nearly full conversion to cycloalkanes (95.6%), oxygen-containing organic compounds (OCOCs, 4.2%), and minor amounts of chain alkanes (CAs, 0.2%). These results collectively point to the pivotal role of both the tailored pore architecture and the uniform distribution of NNPs, which synergistically enhance molecular diffusion, active site accessibility, and the efficiency of hydrocracking and heteroatoms (HAs) removal processes.