The hydrogenation of polycyclic aromatic hydrocarbons (PAHs) over highly efficient and stable catalysts to fine chemicals and intermediates for producing chemical materials is an effective approach to realize the high value-added utilization of coal tar and slurry oil. Herein, two kinds of Al2O3-supported Pt and Rh catalysts are synthesized by strong electrostatic adsorption (SEA) and used to catalyze the hydrogenation of anthracene. Compared with the traditional catalysts synthesized by wet impregnation, the Pt/Al2O3-SEA and Rh/Al2O3-SEA catalysts have smaller active metal particle sizes and higher dispersion, which can expose more active centers, showing higher catalytic activity. Interestingly, anthracene may be preferentially adsorbed on the surface of the Pt/Al2O3 catalyst in a parallel manner but on the surface of the Rh/Al2O3 catalyst in a lateral manner, which leads to the different hydrogenation routes. 9,10-Dihydroanthracene is an initial product for the hydrogenation of anthracene, which is rearranged into tetrahydroanthracene and subsequently hydrogenated to symmetrical octahydroanthracene (sym-OHA) over the Pt/Al2O3 catalyst. The high selectivity to sym-OHA (93%) with the conversion of anthracene near 100% can be achieved in the hydrogenation of anthracene at 240 °C and 7 MPa for 10 h. Additionally, due to the strong anchoring effect, the Pt/Al2O3-SEA catalyst shows high stability for six cycles. This work supplies a new tactic to develop high-performance catalysts for selective hydrogenation of PAHs to important monomers for synthesizing chemical materials.
Interactions between metals and oxide supports are crucial in determining catalytic activity, selectivity, and stability. For reducible oxide supported noble metals, a strong metal–support interaction (SMSI) has been widely recognized. Herein we report the intermediate selectivity and stability over an irreducible SiO2 supported Pt catalyst in the hydrogenation of anthracene that are significantly boosted due to the SMSI-induced formation of intermetallic Pt silicide and Pt–SiO2 interface. The limitation in the strong interaction between Pt nanoparticles and irreducible SiO2 has been breached by combining the strong electrostatic adsorption method and following the high temperature reduction strategy. Due to the isolated Pt active sites by Si atoms, the activated H species produced over the Pt2Si/SiO2 catalyst with an initial catalytic activity of 2.49 μmol/(m2/g)/h as well as TOF of 0.95 s–1 preferentially transfer to the outer ring of anthracene to 87% yield of symmetric octahydroanthracene (sym-OHA) by subsequent hydrogenation. In addition, the Pt2Si/SiO2 catalyst presents an excellent stability after five cycles, which can be attributed to the fact that intermetallic Pt2Si nanoparticles are anchored firmly onto the surface of the SiO2 support. The discovery contributes to broaden the horizons on the SMSI effect in the irreducible oxide supported metal particle catalysts and provides guidance to design the metal–SiO2 interface and tune the surface chemical properties in diverse application conditions.
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